Metal-halide hybrid perovskite materials are excellent candidates for solar cells and photoelectric devices.In recent years,machine learning(ML)techniques have developed rapidly in many fields and provided ideas for m...Metal-halide hybrid perovskite materials are excellent candidates for solar cells and photoelectric devices.In recent years,machine learning(ML)techniques have developed rapidly in many fields and provided ideas for material discovery and design.ML can be applied to discover new materials quickly and effectively,with significant savings in resources and time compared with traditional experiments and density functional theory(DFT)calculations.In this review,we present the application of ML in per-ovskites and briefly review the recent works in the field of ML-assisted perovskite design.Firstly,the advantages of perovskites in solar cells and the merits of ML applied to perovskites are discussed.Secondly,the workflow of ML in perovskite design and some basic ML algorithms are introduced.Thirdly,the applications of ML in predicting various properties of perovskite materials and devices are reviewed.Finally,we propose some prospects for the future development of this field.The rapid devel-opment of ML technology will largely promote the process of materials science,and ML will become an increasingly popular method for predicting the target properties of materials and devices.展开更多
Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active photocathodes.P...Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active photocathodes.Present work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic nanocrystals.When employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging process.Additionally,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky contact.Benefiting from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1) at 0.2 A g^(−1) under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 cycles.These results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.展开更多
Chitosan （CTS） coatings contained calcium （Ca） and phosphorus （P） on titanium （Ti） surface are prepared by the cathode liquid phase plasma technology （CLPT）, in a certain concentration electrolyte solution w...Chitosan （CTS） coatings contained calcium （Ca） and phosphorus （P） on titanium （Ti） surface are prepared by the cathode liquid phase plasma technology （CLPT）, in a certain concentration electrolyte solution with selective additions of ammonium dihydrogen phosphate and calcium nitrate. It is indicated that the parameters for a stable discharge are voltage of 400 V, frequency of 100 Hz, duty cycle of 30% based on a large amount of experiment data. The morphology, structure and composition of the coated samples are studied by SEM, FTIR, XRD, XPS. The results demonstrate that the composite coatings are uniform, and some solid particles of inorganic salt containing calcium and phosphorus dispersed on the coatings. CA tests show that the samples treated by the liquid plasma became less hydrophilic. The variation of hydrophilicity on the CLPT treated titanium is attributed to the change of the function groups on the sample surface. Meanwhile, a possible formation mechanism of the composite coatings is discussed.展开更多
Enhancement of the surface hydrophilicity of biodegradable poly （D,L-lactic acid） （PLA） films is studied. The PLA films were treated by nitrogen plasma （PLA-N2） and nitro- gen/hydrogen plasma （PLA-N2/H2）, resp...Enhancement of the surface hydrophilicity of biodegradable poly （D,L-lactic acid） （PLA） films is studied. The PLA films were treated by nitrogen plasma （PLA-N2） and nitro- gen/hydrogen plasma （PLA-N2/H2）, respectively. The surface properties and microstructure of PLA-N2 and PLA-N2/H2 were studied by static contact angle measurement, surface free energy calculation, X-ray photoelectron spectroscopy （XPS） and atomic force microscopy （AFM）. It is confirmed that the surface hydrophilicity of PLA-N2 and PLA-N2/H2 was higher than that of pristine PLA, and the surface hydrophilicity of PLA-N2 films was better than that of PLA-N2/H2.展开更多
Improving the quality of the perovskite active layer is crucial to obtaining high performance perovskite solar cells(PSCs). In this work, by introducing formic acid into the formamidinium lead iodide(FAPbI3)precursor ...Improving the quality of the perovskite active layer is crucial to obtaining high performance perovskite solar cells(PSCs). In this work, by introducing formic acid into the formamidinium lead iodide(FAPbI3)precursor solution, we managed to achieve reduced colloidal size in the solution, leading to more uniform deposition of FAPbI3 film with lower trap state density and higher carrier mobility. The solar cells based on the FAPbI3 absorber layer modified with formic acid show significantly better photovoltaic performance than that on the reference FAPbI3 film without formic acid. The device performance shows a close correlation with the colloidal size. Within the range studied from 6.7 to 1.0 nm, the smaller the colloidal size is, the higher the solar cell efficiency. More specifically, the cell efficiency is improved from17.82% for the control cell without formic acid to 19.81% when 0.764 M formic acid was used. Formic acid has also been added into a CH3NH3PbI3(MAPbI3) precursor solution, which exhibits a similar effect on the resulting MAPb I3 films and solar cells, with efficiency improved from 16.07% to 17.00%.展开更多
Interface engineering is an effective way to improve efficiency and long-term stability of perovskite solar cells(PSCs).Herein,an ionic compound tetrabutylammonium hexafluorophosphate(TP6)is adopted to passivate surfa...Interface engineering is an effective way to improve efficiency and long-term stability of perovskite solar cells(PSCs).Herein,an ionic compound tetrabutylammonium hexafluorophosphate(TP6)is adopted to passivate surface defects of the perovskite film.It is found that TP6 effectively reduced the surface defects,especially at the grain boundaries where the defects are abundant.Meanwhile,the exposed long alkyl chains and fluorine atoms in the TP6 enhanced the moisture stability of the perovskite film due to its strong hydrophobicity.In addition,the driving force of charge carrier separation and transport is increased by enlarged built-in potential.Consequently,the power conversion efficiency(PCE)of PSCs is significantly improved from 20.59% to 22.41%by increased open-circuit voltage(V_(oc))and fill factor(FF).The unencapsulated device with TP6 treatment exhibits better stability than the control device,and the PCE retains-80%of its initial PCE after 30 days under 15%-25%relative humidity in storage,while the PCE of the control device declines by more than 50%.展开更多
Developing cheap and efficient electrocatalysts for water splitting is required for energy conversion techniques.Many first-row transition metal complexes have been shown to be active for the hydrogen evolution reacti...Developing cheap and efficient electrocatalysts for water splitting is required for energy conversion techniques.Many first-row transition metal complexes have been shown to be active for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Metal ions play crucial roles in these catalytic processes,but the activity dependence on the nature of metal ions has been rarely studied due to the difficulty to compare metal complexes with different coordination environments.We herein reported the synthesis of a series of metal complexes of azido-substituted porphyrin(1),in which metal ions have very similar coordination environments.By grafting 1-M(M=Mn,Fe,Co,Ni,and Cu)onto alkynefunctionalized carbon nanotubes(CNTs)through the same covalent connection,the resulted hybrids 1-M@CNT were all active and robust for both electrocatalytic HER and OER in alkaline aqueous solutions.Among these hybrids,1-Fe@CNT displayed the highest electrocatalytic activity for HER,while 1-Co@CNT was the most active one for OER.Moreover,a two-electrode water electrolysis cell assembled with 1-Fe@CNT as the cathode and 1-Co@CNT as the anode required smaller applied bias potential by210 mV to get 10 mA/cm^(2)current density as compared to that assembled with Pt/C and Ir/C with the same amount of metal loading.This work is significant to correlate HER and OER activity with the nature of first-row transition metal ions and to highlight promising potential applications of molecular electrocatalysis in water splitting.展开更多
The purpose of this paper was to enhance blood compatibility of polyethylene （PE） film. PE film pretreated by argon plasma was subjected to ultraviolet （UV） -induced graft polymerization with Acrylic acid（AAc） ...The purpose of this paper was to enhance blood compatibility of polyethylene （PE） film. PE film pretreated by argon plasma was subjected to ultraviolet （UV） -induced graft polymerization with Acrylic acid（AAc） （AAc-grafted PE films, PE-g-PAAc） without photo-initiator, then heparin was covalently immobilized on the PE surface （PE-g-HPAAc）. The surface properties and microstructure of PE-g-PAAc and PE-g-HPAAc were studied by static contact angle measurement, atomic force microscope （AFM）, X-ray photoelectron spectroscopy （XPS） and Attenuated total reflectance Fourier transfer infrared spectroscopy （ATR-FTIR）. It was confirmed that AAc and heparin were successfully immobilized onto the surface of PE film. Results of platelet adhesion experiments indicated that the antithrombogenicity of the modified PE film was remarkably improved.展开更多
Nickel oxides and(oxy)hydroxides are promising replacements for noble-metal-based catalysts owing to their high activity and good long-term stability for the oxygen evolution reaction(OER). Herein, we developed nanopo...Nickel oxides and(oxy)hydroxides are promising replacements for noble-metal-based catalysts owing to their high activity and good long-term stability for the oxygen evolution reaction(OER). Herein, we developed nanoporous Ni by a method of combined rapid solidification and chemical dealloying. Subsequently,nanoporous Ni O was obtained via heating treatment, the macropore and skeleton sizes of the NiO originated from Ni10Al90 alloy are 100–300 nm and 80–200 nm, respectively. Benefiting from the multi-stage nanoporous structure and high specific surface area, the nanoporous NiO demonstrates an outstanding OER, reaching 20 mA cm-2 at an overpotential of 356 mV in 1 M KOH. The corresponding Tafel slope and apparent activation energy are measured to be 76.73 mV dec-1 and 29.0 kJ mol-1, respectively. Moreover,kinetic analysis indicates that the Ni O catalyst shows pseudocapacitive characteristics, and the improved current is attributed to the high-rate pseudocapacitive behavior that efficiently maintains increased nickel redox cycling to accelerate the reaction rates. After 1000 cycles of voltammetry, the overpotential of the NiO decreases by 22 mV(j = 10 mA cm-2), exhibiting excellent stability and durability.展开更多
Heat transfer is the foundation of freezing colloidal suspensions and a key factor for the interface movement.However,how the thermal conductivity of particles affects freezing microstructural evolution remains unknow...Heat transfer is the foundation of freezing colloidal suspensions and a key factor for the interface movement.However,how the thermal conductivity of particles affects freezing microstructural evolution remains unknown.Here in this work,a mathematical model is built up to investigate thermal interactions among a growing particle layer,pulling speeds,and the freezing interface under a thermal gradient.Experiments are conducted to confirm the tendency predictions of the model.With the increase of pulling speeds,the drifting distance of the freezing interface increases and the time to finish drifting decreases.When the thermal conductivity of particles(k_(p))is smaller than that of the surrounding(kw),the freezing interface tends to go forward to the warm side.Contrarily,the freezing interface tends to go back to the cold side when the thermal conductivity of particles is larger than that of the surrounding(α=k_(p)/k_(w)>1).It originates from the shape of the local freezing interface:convex(α<1)or concave(α>1).These morphological changes in the local interface modify the premelting drag force F_(f).Whenα<1,F_(f)decreases and the freezing morphology tends to be the frozen fringe.Whenα>1,F_(f)increases and the freezing morphologies tend to be ice spears.These understandings of how the thermal conductivity of particles affect microstructural evolution may optimize the production of freeze-casting materials and their structural-functional properties.展开更多
Palladium(Pd) nanostructures are highly promising electrocatalysts for the carbon dioxide electrochemical reduction(CO_(2) ER). At present, it is still challenge for the synthesis of Pd nanostructures with high activi...Palladium(Pd) nanostructures are highly promising electrocatalysts for the carbon dioxide electrochemical reduction(CO_(2) ER). At present, it is still challenge for the synthesis of Pd nanostructures with high activity, selectivity and stability. In this work, a facile PdII-complex pyrolysis method is applied to synthesize the high-quality one-dimensional heterostructured Pd/Pd O nanowires(Pd/Pd O H-NWs).The as-prepared Pd/Pd O H-NWs have a large electrochemically active surface area, abundant defects and Pd/Pd O heterostructure. Electrochemical measurement results reveal that Pd/Pd O H-NWs exhibit up to 94% CO Faraday efficiency with a current density of 11.6 m A cm^(-2) at an applied potential of -0.8 V. Meanwhile, Pd/Pd O H-NWs can achieve a stable catalytic process of 12 h for CO_(2) ER. Such outstanding CO_(2) ER performance of Pd/Pd O H-NWs has also been verified in the flow cell test. The density functional theory calculations indicate that Pd/Pd O heterostructure can significantly weaken the CO adsorption on Pd sites, which improves the CO tolerance and consequently enhances the catalytic performance of Pd/Pd O H-NWs for CO_(2) ER. This work highlights a facile complex pyrolysis strategy for the synthesis of Pd-based CO_(2) ER catalysts and provides a new application instance of metal/metal oxide heterostructure in electrocatalysis.展开更多
Flexible perovskite solar cells(FPSCs) have attracted enormous interest in wearable and portable electronics due to their high power-per-weight and low cost. Flexible and efficient perovskite solar cells require the d...Flexible perovskite solar cells(FPSCs) have attracted enormous interest in wearable and portable electronics due to their high power-per-weight and low cost. Flexible and efficient perovskite solar cells require the development of flexible electrodes compatible with the optoelectronic properties of perovskite. In this review, the recent progress of flexible electrodes used in FPSCs is comprehensively reviewed. The major features of flexible transparent electrodes, including transparent conductive oxides, conductive polymer, carbon nanomaterials and nanostructured metallic materials are systematically compared. And the corresponding modification strategies and device performance are summarized. Moreover, flexible opaque electrodes including metal films, opaque carbon materials and metal foils are critically assessed. Finally, the development directions and difficulties of flexible electrodes are given.展开更多
Two dimensional halide perovskites are emerging as attractive electroluminescent materials for developing high-performance light-emitting devices owing to their unique structures and/or superior optoelectronic propert...Two dimensional halide perovskites are emerging as attractive electroluminescent materials for developing high-performance light-emitting devices owing to their unique structures and/or superior optoelectronic properties.This review begins with an introduction to the working principles of and the key figures for evaluating the performance of LEDs.Secondly,the structure and optoelectronic properties of two dimensional perovskites are summarized and discussed. Their advantages in LED application over their 3D counterparts are systematically analyzed.Following the theoretically discussion,the progresses on the preparation of two dimensional perovskite materials as well as their performances in LEDs have been summarized. At last,several challenges and prospects are presented for achieving high performance 2D perovskite-based LEDs.展开更多
Designing a highly active-and stable non-noble metal bifunctional oxygen catalyst for rechargeable Znair battery remains a great challenge. Herein, we develop a facile and melamine-assisted-pyrolysis(MAP)strategy for ...Designing a highly active-and stable non-noble metal bifunctional oxygen catalyst for rechargeable Znair battery remains a great challenge. Herein, we develop a facile and melamine-assisted-pyrolysis(MAP)strategy for the synthesis of core–shell Co-based electrocatalysts@N-doped carbon nanotubes(Co@CNTs)derived from metal–organic frameworks. The Co@CNTs exhibited excellent bifunctional electrocatalytic performance for both oxygen evolution and reduction. DFT calculations demonstrated that the Gibbs free energy of the rate-determining step was small enough to improve ORR activities. As a result, a Zn-air battery assembled with Co@CNTs proves a lager power density, low voltage gap between charge–discharge and excellent stability. Thus, this work offers a facile strategy to realize the synthesis of non-noble metal electrocatalyst for Zn-air battery materials with high electrochemical performance.展开更多
Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this...Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this work, 1, 10-phenanthroline monohydrate(PM) functionalized Pt nanodendrites(Pt-NDs) on carbon cloth(CC)(denoted as PM@Pt-NDs/CC) and polyethylenimine(PEI) functionalized Pt-NDs on CC(denoted as PEI@Pt-NDs/CC) are successfully achieved by immersing Pt-NDs/CC into PM and PEI aqueous solutions, respectively. PEI functionalization of Pt-NDs/CC improves its electroactivity for hydrogen evolution reaction(HER) due to local proton enrichment whereas PM functionalization of Pt-NDs/CC improves its electroactivity for formic acid oxidation reaction(FAOR) by facilitating dehydrogenation pathway. With such high activity, a two-electrode electrolyzer is assembled using PM@Pt-NDs/CC as the anodic electrocatalyst and PEI@Pt-NDs/CC as the cathodic electrocatalyst for electrochemical reforming of formic acid, which only requires 0.45 V voltage to achieve the current density of 10 mA cm^(-1) for highpurity hydrogen production, much lower than conventional water electrolysis(1.59 V). The work presents an example of interfacial engineering enhancing electrocatalytic activity and indicates that electrochemical reforming of formic acid is an energy-saving electrochemical method for high-purity hydrogen production.展开更多
Perovskite-based tandem solar cells have attracted increasing interest because of its great potential to surpass the Shockley-Queisser limit set for single-junction solar cells.In the tandem architectures,the wide-ban...Perovskite-based tandem solar cells have attracted increasing interest because of its great potential to surpass the Shockley-Queisser limit set for single-junction solar cells.In the tandem architectures,the wide-bandgap(WBG)perovskites act as the front absorber to offer higher open-circuit voltage(VOC)for reduced thermalization losses.Taking advantage of tunable bandgap of the perovskite materials,the WBG perovskites can be easily obtained by substituting halide iodine with bromine,and substituting organic ions FA and MA with Cs.To date,the most concerned issues for the WBG perovskite solar cells(PSCs)are huge VOC deficit and severe photo-induced phase separation.Reducing VOC loss and improving photostability of the WBG PSCs are crucial for further efficiency breakthrough.Recently,scientists have made great efforts to overcome these key issues with tremendous progresses.In this review,we first summarize the recent progress of WBG perovskites from the aspects of compositions,additives,charge transport layers,interfaces and preparation methods.The key factors affecting efficiency and stability are then carefully discussed,which would provide decent guidance to develop highly efficient and stable WBG PSCs for tandem application.展开更多
Transition-metal based M-N_4/C catalysts are appealing for electrocatalytic oxygen reduction reaction(ORR) and oxygen evolution reaction(OER). Employing model catalysts, which have well-defined molecular structures an...Transition-metal based M-N_4/C catalysts are appealing for electrocatalytic oxygen reduction reaction(ORR) and oxygen evolution reaction(OER). Employing model catalysts, which have well-defined molecular structures and coordination environments, to investigate electrocatalytic performance of M-N_4/C sites for ORR and OER is of fundamental significance. Herein, we reported the use of Co tetra(phenyl)porphyrin 1 and Co tetra(pentafluorophenyl)porphyrin 2 as models to probe the role of Co-N_4/C sites for oxygen electrocatalysis. We showed that Co porphyrin 1 is more efficient than its structural analogue 2 for oxygen electrocatalysis in alkaline aqueous solutions, indicating that the electronrich Co-N_4/C site is more favored when noncovalently adsorbed on carbon supports. This work inspires rational design of reaction-oriented catalysts for sustainable energy storage and conversion technologies.展开更多
Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries(GBs)of perovskite materials for enhanced photovoltaic performance and stability of perovskite so...Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries(GBs)of perovskite materials for enhanced photovoltaic performance and stability of perovskite solar cells(PSCs).Here,(BBF)complex is chosen as a multifunctional additive,which contains both C7H9N and BF3 groups working as Lewis base and Lewis acid,respectively,can bond with Pb^(2+)/I^(−) and FA+on the surface and in the GBs in the perovskite film,affording passivation of both cation and anion defects.The synergistic effect of the C7H9N and BF3 complex slows the crystallization during the perovskite film deposition to improve the crystalline quality,which reduces the trap density and the recombination in the perovskite film to suppress nonradiative recombination loss and minimizes moisture permeation to improve the stability of the perovskite material.Meanwhile,such an additive improves the energy-level alignment between the valence band of the perovskite and the highest occupied molecular orbital of the hole-transporting material,Spiro-OMeTAD.Consequently,our work achieves power conversion efficiency of 23.24%,accompanied by enhanced stability under ambient conditions and light illumination and opens a new avenue for improving the performance of PSCs through the use of a multifunctional complex.展开更多
Here we exquisitely fabricated Cu/ZrO_(2)-dp catalysts with plentiful Cu-ZrO_(2)interfaces by depositing amorphous ZrO_(2)onto Cu nanoparticles for the hydrogenation of levulinic acid(LA)to y-valerolactone(GVL).With t...Here we exquisitely fabricated Cu/ZrO_(2)-dp catalysts with plentiful Cu-ZrO_(2)interfaces by depositing amorphous ZrO_(2)onto Cu nanoparticles for the hydrogenation of levulinic acid(LA)to y-valerolactone(GVL).With the created plentiful CU-ZrO_(2)interfaces,the optimal catalyst 3 Cu/ZrO_(2)-dp exhibited exceptional catalytic performance under mild reaction conditions,and achieved the highest GVL mass productivity of 266.0 mmol GVL·h^(-1)·g^(-1)Cu,which was 12.5 and 2.3 times of CU/ZrO_(2)catalysts with equivalent Cu loadings prepared by traditional impregnation(3 Cu/ZrO_(2)-im)or co-precipitation(3 Cu/ZrO_(2)-cp).As far as we know,this GVL mass productivity stood at the highest level compared with those obtained using non-noble metal catalysts under similar reaction conditions.By systematic investigation with multiple characterizations,density functional theory(DFT)calculations,and kinetic studies,it was found that interfacial active centers were created at Cu-ZrO_(2)interfaces,which contained oxygen vacancies(O_(v)),negatively charged Cu^(δ)-and partially reduced Zr^(3+)The O_(v) favored the adsorption and activation of LA via its ketone group,while negatively charged Cu^(δ)-was able to enhance heterolysis of H2,which resulted in the formation of H^(+)-Cu^(δ)-and Zr^(3+)-H^(-)active species via hydrogen spillover.Also,plentiful acid sites,which derived from coordinatively unsaturated and defective Zr species,generated at Cu-ZrO_(2)interfaces.With the cooperation of interfacial active centers(Cu^(δ-)-O_(v)-Zr^(3+))and acid sites,the fabricated 3 Cu/ZrO_(2)-dp with plentiful Cu-ZrO_(2)interfaces achieved excellent catalytic performance for the hydrogenation of LA to GVL.Hence,the synergistic catalysis of Cu-ZrO_(2)interfaces provided an effective strategy for designing catalysts with a satisfactory performance for the hydrogenation of LA,which also can be expanded to other hydrodeoxygenation reactions.展开更多
The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement rema...The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.展开更多
基金funded by the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No.XDA17040506)the National Natural Science Foundation of China(62005148/12004235)+2 种基金The Open Competition Mechanism to Select The Best Candidates Project in Jinzhong Science and Technology Bureau (J202101)the DNL Cooperation Fund CAS(DNL180311)the 111 Project (B14041)
文摘Metal-halide hybrid perovskite materials are excellent candidates for solar cells and photoelectric devices.In recent years,machine learning(ML)techniques have developed rapidly in many fields and provided ideas for material discovery and design.ML can be applied to discover new materials quickly and effectively,with significant savings in resources and time compared with traditional experiments and density functional theory(DFT)calculations.In this review,we present the application of ML in per-ovskites and briefly review the recent works in the field of ML-assisted perovskite design.Firstly,the advantages of perovskites in solar cells and the merits of ML applied to perovskites are discussed.Secondly,the workflow of ML in perovskite design and some basic ML algorithms are introduced.Thirdly,the applications of ML in predicting various properties of perovskite materials and devices are reviewed.Finally,we propose some prospects for the future development of this field.The rapid devel-opment of ML technology will largely promote the process of materials science,and ML will become an increasingly popular method for predicting the target properties of materials and devices.
基金supported by the project of the National Natural Science Foundation of China(52202115 and 52172101)Guangdong Basic and Applied Basic Research Foundation(2024A1515012325)+2 种基金the Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX1085)the Shaanxi Science and Technology Innovation Team(2023-CXTD-44)the Fundamental Research Funds for the Central Universities(G2022KY0604).
文摘Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active photocathodes.Present work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic nanocrystals.When employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging process.Additionally,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky contact.Benefiting from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1) at 0.2 A g^(−1) under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 cycles.These results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.
基金supported by National Natural Science Foundation of China (No.10675078)
文摘Chitosan （CTS） coatings contained calcium （Ca） and phosphorus （P） on titanium （Ti） surface are prepared by the cathode liquid phase plasma technology （CLPT）, in a certain concentration electrolyte solution with selective additions of ammonium dihydrogen phosphate and calcium nitrate. It is indicated that the parameters for a stable discharge are voltage of 400 V, frequency of 100 Hz, duty cycle of 30% based on a large amount of experiment data. The morphology, structure and composition of the coated samples are studied by SEM, FTIR, XRD, XPS. The results demonstrate that the composite coatings are uniform, and some solid particles of inorganic salt containing calcium and phosphorus dispersed on the coatings. CA tests show that the samples treated by the liquid plasma became less hydrophilic. The variation of hydrophilicity on the CLPT treated titanium is attributed to the change of the function groups on the sample surface. Meanwhile, a possible formation mechanism of the composite coatings is discussed.
基金supported by the Fundamental Research Funds for the Central Universities (Nos. GK200901023, GK201004001)
文摘Enhancement of the surface hydrophilicity of biodegradable poly （D,L-lactic acid） （PLA） films is studied. The PLA films were treated by nitrogen plasma （PLA-N2） and nitro- gen/hydrogen plasma （PLA-N2/H2）, respectively. The surface properties and microstructure of PLA-N2 and PLA-N2/H2 were studied by static contact angle measurement, surface free energy calculation, X-ray photoelectron spectroscopy （XPS） and atomic force microscopy （AFM）. It is confirmed that the surface hydrophilicity of PLA-N2 and PLA-N2/H2 was higher than that of pristine PLA, and the surface hydrophilicity of PLA-N2 films was better than that of PLA-N2/H2.
基金supported by the National Key Research and Development Program of China(NO.2016YFA0202403/2017YFA0204800)the National Natural Science Foundation of China(61604091 and 61674098)+3 种基金the 111 Project(B14041)the National University Research Fund(Grant Nos.GK261001009,GK201603107)the Changjiang Scholar and Innovative Research Team(IRT_14R33)the Chinese National 1000-talent-plan program(1110010341)。
文摘Improving the quality of the perovskite active layer is crucial to obtaining high performance perovskite solar cells(PSCs). In this work, by introducing formic acid into the formamidinium lead iodide(FAPbI3)precursor solution, we managed to achieve reduced colloidal size in the solution, leading to more uniform deposition of FAPbI3 film with lower trap state density and higher carrier mobility. The solar cells based on the FAPbI3 absorber layer modified with formic acid show significantly better photovoltaic performance than that on the reference FAPbI3 film without formic acid. The device performance shows a close correlation with the colloidal size. Within the range studied from 6.7 to 1.0 nm, the smaller the colloidal size is, the higher the solar cell efficiency. More specifically, the cell efficiency is improved from17.82% for the control cell without formic acid to 19.81% when 0.764 M formic acid was used. Formic acid has also been added into a CH3NH3PbI3(MAPbI3) precursor solution, which exhibits a similar effect on the resulting MAPb I3 films and solar cells, with efficiency improved from 16.07% to 17.00%.
基金funded by the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDA17040506)the National Key Research and Development Program of China (2017YFA0204800/2016YFA0202403)+6 种基金the Key Program project of the National Natural Science Foundation of China (51933010)the National Natural Science Foundation of China (61974085)the 111 Project (B21005)the Changjiang Scholars and Innovative Research Team (IRT_14R33)the National University Research Fund (GK201903051)the Research Start-up Fund from Shaanxi Normal University (1110020142)the Shanxi Science and Technology Department (20201101012).
文摘Interface engineering is an effective way to improve efficiency and long-term stability of perovskite solar cells(PSCs).Herein,an ionic compound tetrabutylammonium hexafluorophosphate(TP6)is adopted to passivate surface defects of the perovskite film.It is found that TP6 effectively reduced the surface defects,especially at the grain boundaries where the defects are abundant.Meanwhile,the exposed long alkyl chains and fluorine atoms in the TP6 enhanced the moisture stability of the perovskite film due to its strong hydrophobicity.In addition,the driving force of charge carrier separation and transport is increased by enlarged built-in potential.Consequently,the power conversion efficiency(PCE)of PSCs is significantly improved from 20.59% to 22.41%by increased open-circuit voltage(V_(oc))and fill factor(FF).The unencapsulated device with TP6 treatment exhibits better stability than the control device,and the PCE retains-80%of its initial PCE after 30 days under 15%-25%relative humidity in storage,while the PCE of the control device declines by more than 50%.
基金support from the Fok Ying-Tong Education Foundation for Outstanding Young Teachers in Universitythe National Natural Science Foundation of China(21773146)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Research Funds of Shaanxi Normal University。
文摘Developing cheap and efficient electrocatalysts for water splitting is required for energy conversion techniques.Many first-row transition metal complexes have been shown to be active for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Metal ions play crucial roles in these catalytic processes,but the activity dependence on the nature of metal ions has been rarely studied due to the difficulty to compare metal complexes with different coordination environments.We herein reported the synthesis of a series of metal complexes of azido-substituted porphyrin(1),in which metal ions have very similar coordination environments.By grafting 1-M(M=Mn,Fe,Co,Ni,and Cu)onto alkynefunctionalized carbon nanotubes(CNTs)through the same covalent connection,the resulted hybrids 1-M@CNT were all active and robust for both electrocatalytic HER and OER in alkaline aqueous solutions.Among these hybrids,1-Fe@CNT displayed the highest electrocatalytic activity for HER,while 1-Co@CNT was the most active one for OER.Moreover,a two-electrode water electrolysis cell assembled with 1-Fe@CNT as the cathode and 1-Co@CNT as the anode required smaller applied bias potential by210 mV to get 10 mA/cm^(2)current density as compared to that assembled with Pt/C and Ir/C with the same amount of metal loading.This work is significant to correlate HER and OER activity with the nature of first-row transition metal ions and to highlight promising potential applications of molecular electrocatalysis in water splitting.
基金National Natural Science Foundation of China(No.10675078)
文摘The purpose of this paper was to enhance blood compatibility of polyethylene （PE） film. PE film pretreated by argon plasma was subjected to ultraviolet （UV） -induced graft polymerization with Acrylic acid（AAc） （AAc-grafted PE films, PE-g-PAAc） without photo-initiator, then heparin was covalently immobilized on the PE surface （PE-g-HPAAc）. The surface properties and microstructure of PE-g-PAAc and PE-g-HPAAc were studied by static contact angle measurement, atomic force microscope （AFM）, X-ray photoelectron spectroscopy （XPS） and Attenuated total reflectance Fourier transfer infrared spectroscopy （ATR-FTIR）. It was confirmed that AAc and heparin were successfully immobilized onto the surface of PE film. Results of platelet adhesion experiments indicated that the antithrombogenicity of the modified PE film was remarkably improved.
基金the funding support from the National Natural Science Foundation of China(No.51661018)the support from National Key Research Program of China(2017YFA0204800,2016YFA0202403)+3 种基金Natural Science Foundation of China(No.21603136)the National Science Basic Research Plan in Shaanxi Province of China(2017JM2007)the Changjiang Scholar and Innovative Research Team(IRT_14R33)The 111 Project(B14041)。
文摘Nickel oxides and(oxy)hydroxides are promising replacements for noble-metal-based catalysts owing to their high activity and good long-term stability for the oxygen evolution reaction(OER). Herein, we developed nanoporous Ni by a method of combined rapid solidification and chemical dealloying. Subsequently,nanoporous Ni O was obtained via heating treatment, the macropore and skeleton sizes of the NiO originated from Ni10Al90 alloy are 100–300 nm and 80–200 nm, respectively. Benefiting from the multi-stage nanoporous structure and high specific surface area, the nanoporous NiO demonstrates an outstanding OER, reaching 20 mA cm-2 at an overpotential of 356 mV in 1 M KOH. The corresponding Tafel slope and apparent activation energy are measured to be 76.73 mV dec-1 and 29.0 kJ mol-1, respectively. Moreover,kinetic analysis indicates that the Ni O catalyst shows pseudocapacitive characteristics, and the improved current is attributed to the high-rate pseudocapacitive behavior that efficiently maintains increased nickel redox cycling to accelerate the reaction rates. After 1000 cycles of voltammetry, the overpotential of the NiO decreases by 22 mV(j = 10 mA cm-2), exhibiting excellent stability and durability.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2018YFB1106003,2017YFA0204800,and2016YFA0202403)the National Natural Science Foundation of China(Grant No.51901190)+1 种基金the China Postdoctoral Science Foundation(Grant No.2020M673336)the Peak Experience Program(2018)of Northwestern Polytechnical University,China。
文摘Heat transfer is the foundation of freezing colloidal suspensions and a key factor for the interface movement.However,how the thermal conductivity of particles affects freezing microstructural evolution remains unknown.Here in this work,a mathematical model is built up to investigate thermal interactions among a growing particle layer,pulling speeds,and the freezing interface under a thermal gradient.Experiments are conducted to confirm the tendency predictions of the model.With the increase of pulling speeds,the drifting distance of the freezing interface increases and the time to finish drifting decreases.When the thermal conductivity of particles(k_(p))is smaller than that of the surrounding(kw),the freezing interface tends to go forward to the warm side.Contrarily,the freezing interface tends to go back to the cold side when the thermal conductivity of particles is larger than that of the surrounding(α=k_(p)/k_(w)>1).It originates from the shape of the local freezing interface:convex(α<1)or concave(α>1).These morphological changes in the local interface modify the premelting drag force F_(f).Whenα<1,F_(f)decreases and the freezing morphology tends to be the frozen fringe.Whenα>1,F_(f)increases and the freezing morphologies tend to be ice spears.These understandings of how the thermal conductivity of particles affect microstructural evolution may optimize the production of freeze-casting materials and their structural-functional properties.
基金supported by the National Natural Science Foundation of China(51873100)Natural Science Foundation of Shaanxi Province(2020JZ-23)+2 种基金the Fundamental Research Funds for the Central Universities(GK202101005 and 2021CBLZ004)the Innovation Team Project for Graduate Student at Shaanxi Normal University(TD2020048Y)the 111 Project(B14041)。
文摘Palladium(Pd) nanostructures are highly promising electrocatalysts for the carbon dioxide electrochemical reduction(CO_(2) ER). At present, it is still challenge for the synthesis of Pd nanostructures with high activity, selectivity and stability. In this work, a facile PdII-complex pyrolysis method is applied to synthesize the high-quality one-dimensional heterostructured Pd/Pd O nanowires(Pd/Pd O H-NWs).The as-prepared Pd/Pd O H-NWs have a large electrochemically active surface area, abundant defects and Pd/Pd O heterostructure. Electrochemical measurement results reveal that Pd/Pd O H-NWs exhibit up to 94% CO Faraday efficiency with a current density of 11.6 m A cm^(-2) at an applied potential of -0.8 V. Meanwhile, Pd/Pd O H-NWs can achieve a stable catalytic process of 12 h for CO_(2) ER. Such outstanding CO_(2) ER performance of Pd/Pd O H-NWs has also been verified in the flow cell test. The density functional theory calculations indicate that Pd/Pd O heterostructure can significantly weaken the CO adsorption on Pd sites, which improves the CO tolerance and consequently enhances the catalytic performance of Pd/Pd O H-NWs for CO_(2) ER. This work highlights a facile complex pyrolysis strategy for the synthesis of Pd-based CO_(2) ER catalysts and provides a new application instance of metal/metal oxide heterostructure in electrocatalysis.
基金financially supported by the National Natural Science Foundation of China(52192610)the National Key Research and Development Program of China(Grant 2021YFA0715600)+1 种基金the Key Research and Development Program of Shaanxi Province(Grant 2020GY-310)the Fundamental Research Funds for the Central Universities and the Innovation Fund of Xidian University。
文摘Flexible perovskite solar cells(FPSCs) have attracted enormous interest in wearable and portable electronics due to their high power-per-weight and low cost. Flexible and efficient perovskite solar cells require the development of flexible electrodes compatible with the optoelectronic properties of perovskite. In this review, the recent progress of flexible electrodes used in FPSCs is comprehensively reviewed. The major features of flexible transparent electrodes, including transparent conductive oxides, conductive polymer, carbon nanomaterials and nanostructured metallic materials are systematically compared. And the corresponding modification strategies and device performance are summarized. Moreover, flexible opaque electrodes including metal films, opaque carbon materials and metal foils are critically assessed. Finally, the development directions and difficulties of flexible electrodes are given.
基金funded by the National Key Research and Development Program of China (2017YFA0204800/2016YFA0202403)the Fundamental Research Funds for the Central Universities (2018CBLZ006)+3 种基金National Natural Science Foundation of China (61604091 and 61674098)the 111 Project (B14041)the Changjiang Scholar and Innovative Research Team (IRT_14R33)the Chinese National 1000-talent-plan program (1110010341)
文摘Two dimensional halide perovskites are emerging as attractive electroluminescent materials for developing high-performance light-emitting devices owing to their unique structures and/or superior optoelectronic properties.This review begins with an introduction to the working principles of and the key figures for evaluating the performance of LEDs.Secondly,the structure and optoelectronic properties of two dimensional perovskites are summarized and discussed. Their advantages in LED application over their 3D counterparts are systematically analyzed.Following the theoretically discussion,the progresses on the preparation of two dimensional perovskite materials as well as their performances in LEDs have been summarized. At last,several challenges and prospects are presented for achieving high performance 2D perovskite-based LEDs.
基金supported by the National Natural Science Foundation of China (51403114, 21905167)Science and Technology Innovation Program of Universities of Shandong Province (2020KJA012)+3 种基金Taishan Scholars Program of Shandong Province (tsqn201909065)China Postdoctoral Science Foundation (No. 2014 M56053, 2019M650232)the Opening Fund of State Key Laboratory of Heavy Oil Processing (SKLOP202002004)Fundamental Research Funds for the Central Universities (GK202003025)。
文摘Designing a highly active-and stable non-noble metal bifunctional oxygen catalyst for rechargeable Znair battery remains a great challenge. Herein, we develop a facile and melamine-assisted-pyrolysis(MAP)strategy for the synthesis of core–shell Co-based electrocatalysts@N-doped carbon nanotubes(Co@CNTs)derived from metal–organic frameworks. The Co@CNTs exhibited excellent bifunctional electrocatalytic performance for both oxygen evolution and reduction. DFT calculations demonstrated that the Gibbs free energy of the rate-determining step was small enough to improve ORR activities. As a result, a Zn-air battery assembled with Co@CNTs proves a lager power density, low voltage gap between charge–discharge and excellent stability. Thus, this work offers a facile strategy to realize the synthesis of non-noble metal electrocatalyst for Zn-air battery materials with high electrochemical performance.
基金sponsored by Natural Science Foundation of Shaanxi Province (2020JZ-23)the Fundamental Research Funds for the Central Universities (GK201901002, GK201701007 and GK201902014)the 111 Project (B14041)。
文摘Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this work, 1, 10-phenanthroline monohydrate(PM) functionalized Pt nanodendrites(Pt-NDs) on carbon cloth(CC)(denoted as PM@Pt-NDs/CC) and polyethylenimine(PEI) functionalized Pt-NDs on CC(denoted as PEI@Pt-NDs/CC) are successfully achieved by immersing Pt-NDs/CC into PM and PEI aqueous solutions, respectively. PEI functionalization of Pt-NDs/CC improves its electroactivity for hydrogen evolution reaction(HER) due to local proton enrichment whereas PM functionalization of Pt-NDs/CC improves its electroactivity for formic acid oxidation reaction(FAOR) by facilitating dehydrogenation pathway. With such high activity, a two-electrode electrolyzer is assembled using PM@Pt-NDs/CC as the anodic electrocatalyst and PEI@Pt-NDs/CC as the cathodic electrocatalyst for electrochemical reforming of formic acid, which only requires 0.45 V voltage to achieve the current density of 10 mA cm^(-1) for highpurity hydrogen production, much lower than conventional water electrolysis(1.59 V). The work presents an example of interfacial engineering enhancing electrocatalytic activity and indicates that electrochemical reforming of formic acid is an energy-saving electrochemical method for high-purity hydrogen production.
基金support from the 111 Project(B21005)the National Natural Science Foundation of China(Grant No.62174103)the National University Research Fund(GK202103108)。
文摘Perovskite-based tandem solar cells have attracted increasing interest because of its great potential to surpass the Shockley-Queisser limit set for single-junction solar cells.In the tandem architectures,the wide-bandgap(WBG)perovskites act as the front absorber to offer higher open-circuit voltage(VOC)for reduced thermalization losses.Taking advantage of tunable bandgap of the perovskite materials,the WBG perovskites can be easily obtained by substituting halide iodine with bromine,and substituting organic ions FA and MA with Cs.To date,the most concerned issues for the WBG perovskite solar cells(PSCs)are huge VOC deficit and severe photo-induced phase separation.Reducing VOC loss and improving photostability of the WBG PSCs are crucial for further efficiency breakthrough.Recently,scientists have made great efforts to overcome these key issues with tremendous progresses.In this review,we first summarize the recent progress of WBG perovskites from the aspects of compositions,additives,charge transport layers,interfaces and preparation methods.The key factors affecting efficiency and stability are then carefully discussed,which would provide decent guidance to develop highly efficient and stable WBG PSCs for tandem application.
基金supported by the "Thousand Talents Program" of China, the Fok Ying-Tong Education Foundation for Outstanding Young Teachers in University, the National Natural Science Foundation of China (21573139, 21773146, 21902099, and 21905167)theChinaPostdoctoralScienceFoundation (2019M650232)+2 种基金the Fundamental Research Funds for the Central Universities (GK202003025)the Research Funds of Shaanxi Normal Universitythe Opening Fund of State Key Laboratory of Heavy Oil Processing。
文摘Transition-metal based M-N_4/C catalysts are appealing for electrocatalytic oxygen reduction reaction(ORR) and oxygen evolution reaction(OER). Employing model catalysts, which have well-defined molecular structures and coordination environments, to investigate electrocatalytic performance of M-N_4/C sites for ORR and OER is of fundamental significance. Herein, we reported the use of Co tetra(phenyl)porphyrin 1 and Co tetra(pentafluorophenyl)porphyrin 2 as models to probe the role of Co-N_4/C sites for oxygen electrocatalysis. We showed that Co porphyrin 1 is more efficient than its structural analogue 2 for oxygen electrocatalysis in alkaline aqueous solutions, indicating that the electronrich Co-N_4/C site is more favored when noncovalently adsorbed on carbon supports. This work inspires rational design of reaction-oriented catalysts for sustainable energy storage and conversion technologies.
基金The authors acknowledge support from the National Natural Science Foundation of China(62074095/61704101/91733301)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities GK(201903048)the 111 Project(Grant No.B21005)the Fundament Research Funds for the Central University(2019TS004)DNL Cooperation Fund CAS(DNL180311).
文摘Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries(GBs)of perovskite materials for enhanced photovoltaic performance and stability of perovskite solar cells(PSCs).Here,(BBF)complex is chosen as a multifunctional additive,which contains both C7H9N and BF3 groups working as Lewis base and Lewis acid,respectively,can bond with Pb^(2+)/I^(−) and FA+on the surface and in the GBs in the perovskite film,affording passivation of both cation and anion defects.The synergistic effect of the C7H9N and BF3 complex slows the crystallization during the perovskite film deposition to improve the crystalline quality,which reduces the trap density and the recombination in the perovskite film to suppress nonradiative recombination loss and minimizes moisture permeation to improve the stability of the perovskite material.Meanwhile,such an additive improves the energy-level alignment between the valence band of the perovskite and the highest occupied molecular orbital of the hole-transporting material,Spiro-OMeTAD.Consequently,our work achieves power conversion efficiency of 23.24%,accompanied by enhanced stability under ambient conditions and light illumination and opens a new avenue for improving the performance of PSCs through the use of a multifunctional complex.
基金financial support from the National Natural Science Foundation of China(21576161,21703133,21802076,and 21962013)the Fundamental Research Funds for the Central Universities(GK202003028)。
文摘Here we exquisitely fabricated Cu/ZrO_(2)-dp catalysts with plentiful Cu-ZrO_(2)interfaces by depositing amorphous ZrO_(2)onto Cu nanoparticles for the hydrogenation of levulinic acid(LA)to y-valerolactone(GVL).With the created plentiful CU-ZrO_(2)interfaces,the optimal catalyst 3 Cu/ZrO_(2)-dp exhibited exceptional catalytic performance under mild reaction conditions,and achieved the highest GVL mass productivity of 266.0 mmol GVL·h^(-1)·g^(-1)Cu,which was 12.5 and 2.3 times of CU/ZrO_(2)catalysts with equivalent Cu loadings prepared by traditional impregnation(3 Cu/ZrO_(2)-im)or co-precipitation(3 Cu/ZrO_(2)-cp).As far as we know,this GVL mass productivity stood at the highest level compared with those obtained using non-noble metal catalysts under similar reaction conditions.By systematic investigation with multiple characterizations,density functional theory(DFT)calculations,and kinetic studies,it was found that interfacial active centers were created at Cu-ZrO_(2)interfaces,which contained oxygen vacancies(O_(v)),negatively charged Cu^(δ)-and partially reduced Zr^(3+)The O_(v) favored the adsorption and activation of LA via its ketone group,while negatively charged Cu^(δ)-was able to enhance heterolysis of H2,which resulted in the formation of H^(+)-Cu^(δ)-and Zr^(3+)-H^(-)active species via hydrogen spillover.Also,plentiful acid sites,which derived from coordinatively unsaturated and defective Zr species,generated at Cu-ZrO_(2)interfaces.With the cooperation of interfacial active centers(Cu^(δ-)-O_(v)-Zr^(3+))and acid sites,the fabricated 3 Cu/ZrO_(2)-dp with plentiful Cu-ZrO_(2)interfaces achieved excellent catalytic performance for the hydrogenation of LA to GVL.Hence,the synergistic catalysis of Cu-ZrO_(2)interfaces provided an effective strategy for designing catalysts with a satisfactory performance for the hydrogenation of LA,which also can be expanded to other hydrodeoxygenation reactions.
基金support from the National Natural Science Foundation of China(62074095)the National Key Research and Development Program of China(2016YFA0202403)+3 种基金the Fundamental Research Funds for the Central Universities(GK202002001)the 111 Project(Grant No.B21005)the DNL Cooperation Fund CAS(DNL180311)the support of H2 cluster in Xi’an Jiaotong University.
文摘The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells(PSCs).However,the detailed mechanisms behind the improvement remain mysterious.Herein,a series of imidazolium-based ionic liquids(IILs)with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites.It is found that IILs display the following advantages:(1)They form ionic bonds with Cs^(+)and Pb^(2+)cations on the surface and at the grain boundaries of perovskite films,which could effectively heal/reduce the Cs^(+)/I−vacancies and Pb-related defects;(2)They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer;and(3)They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI_(2)Br PSCs.The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI_(2)Br PSCs and an impressive power conversion efficiency of 17.02%.Additionally,the CsPbI_(2)Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability.Our results provide guidance for an indepth understanding of the passivation mechanism of IILs in inorganic perovskites.
