Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept ...Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.展开更多
Organometallic halide perovskite materials make great achievements in optoelectronic fields,especially in solar cells,in which the organic cations contain amine components.However,the amine with NàH bonds is easi...Organometallic halide perovskite materials make great achievements in optoelectronic fields,especially in solar cells,in which the organic cations contain amine components.However,the amine with NàH bonds is easily hydrolyzed with moisture in the air,weakening the perovskite materials stability.It is desirable to develop other non-amine stable perovskite materials.In this work,sulfur-based perovskite-like(CH_(3))_(3)SPbI_(3) nanorod arrays were fabricated by a solution-processed method,which can be indexed hexagonal crystal structure in the space group P63 mc.The binding force is exceptionally strong between the non-amine(CH_(3))_(3) S+and[PbI_(6)]_(4)-octahedral,leading to high stability of(CH_(3))_(3)SPbI_(3).The(CH_(3))_(3)SPbI_(3) nanorod arrays can keep the morphology and crystal structure in an ambient atmosphere over 60 days.In addition,the(CH_(3))_(3)SPbI_(3) nanorod arrays can offer direct charge transfer channels,which show excellent optoelectronic properties.The(CH_(3))_(3)SPbI_(3) nanorod arrays-based solar cells with VOx hole transfer layers achieved a power conversion efficiency of 2.07%with negligible hysteresis.And the(CH_(3))_(3)SPbI_(3) nanorod arrays were also effectively applied in photodetectors with interdigitated gold electrodes.This work demonstrates that sulfur-based perovskite-like(CH_(3))_(3)SPbI_(3) is a novel promising stable compound with great potential for practical optoelectronic applications.展开更多
Betavoltaic cells(BCs)are promising self-generating power cells with long life and high power density.However,the low energy conversion efficiency(ECE)has limitations in practical engineering applications.Widebandgap ...Betavoltaic cells(BCs)are promising self-generating power cells with long life and high power density.However,the low energy conversion efficiency(ECE)has limitations in practical engineering applications.Widebandgap semiconductors(WBGSs)with three-dimensional(3-D)nanostructures are ideal candidates for increasing the ECE of BCs.This paper proposes hydrothermally grown ZnO nanorod arrays(ZNRAs)for ^(63)Ni-powered BCs.A quantitative model was established for simulation using the parameter values of the dark characteristics,which were obtained from the experimental measurements for a simulated BC based on a Ni-incorporated ZNRAs structure.Monte Carlo(MC)modeling and simulation were conducted to obtain the values of the β energy deposited in ZNRAs with different nanorod spacings and heights.Through the simulation and optimization of the 3-D ZNRAs and 2-D ZnO bulk structures,the performance of the ^(63)Ni-powered BCs based on both structures was evaluated using a quantitative model.The BCs based on the 3-D ZNRAs structure and 2-D ZnO bulk structure achieved a maximum ECE of 10.1%and 4.69%,respectively,which indicates the significant superiority of 3-D nanostructured WBGSs in increasing the ECE of BCs.展开更多
All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a di...All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a direct Z-scheme photoelectrocatalytic electrode based on a WO_(3-x)nanowire-bridged TiO_(2)nanorod array heterojunction is constructed for overall water splitting,producing H_(2).The as-prepared WO_(3-x)/TiO_(2)nanorod array heterojunction shows photoelectrochemical(PEC)overall water splitting activity evolving both H_(2) and O_(2)under UV-vis light irradiation.An optimum PEC activity was achieved over a 1.67-WO_(3-x)/TiO_(2)photoelectrode yielding maximum H_(2) and O_(2)evolution rates roughly 11 times higher than that of pure TiO_(2)nanorods without any sacrificial agent or redox mediator.The role of oxygen vacancy in WO_(3-x)in affecting the H_(2) production rate was also comprehensively studied.The superior PEC activity of the WO_(3-x)/TiO_(2)electrode for overall water splitting can be ascribed to an efficient Z-scheme charge transfer pathway between the WO_(3-x)nanowires and TiO_(2)nanorods,the presence of oxygen vacancies in WO_(3-x),and a bias potential applied on the photoelectrode,resulting in effective spatial charge separation.This study provides a novel strategy for developing highly efficient PECs for overall water splitting.展开更多
InGaN/GaN epilayers, which are grown on sapphire substrates by the metal-organic chemical-vapour deposition （MOCVD） method, are formed into nanorod arrays using inductively coupled plasma etching via self-assembled ...InGaN/GaN epilayers, which are grown on sapphire substrates by the metal-organic chemical-vapour deposition （MOCVD） method, are formed into nanorod arrays using inductively coupled plasma etching via self-assembled Ni nanomasks. The formation of nanorod arrays eliminates the tilt of the InGaN （0002） crystallographic plane with respect to its GaN bulk layer. Photoluminescence results show an apparent S-shaped dependence on temperature. The light extraction efficiency and intensity of photoluminescence emission at low temperature of less than 30 K for the nanorod arrays are enhanced by the large surface area, which increases the quenching effect because of the high density of surface states for the temperature above 30 K. Additionally, a red-shift for the InGaN/GaN nanorod arrays is observed due to the strain relaxation, which is confirmed by reciprocal space mapping measurements.展开更多
van der Waals(vdW)heterostructures constructed by lowdimensional(0D,1D,and 2D)materials are emerging as one of the most appealing systems in next-generation flexible photodetection.Currently,hand-stacked vdW-type phot...van der Waals(vdW)heterostructures constructed by lowdimensional(0D,1D,and 2D)materials are emerging as one of the most appealing systems in next-generation flexible photodetection.Currently,hand-stacked vdW-type photodetectors are not compatible with large-areaarray fabrication and show unimpressive performance in self-powered mode.Herein,vertical 1D GaN nanorods arrays(NRAs)/2D MoS_(2)/PEDOT:PSS in wafer scale have been proposed for self-powered flexible photodetectors arrays firstly.The as-integrated device without external bias under weak UV illumination exhibits a competitive responsivity of 1.47 A W^(−1)and a high detectivity of 1.2×10^(11)Jones,as well as a fast response speed of 54/71μs,thanks to the strong light absorption of GaN NRAs and the efficient photogenerated carrier separation in type-II heterojunction.Notably,the strain-tunable photodetection performances of device have been demonstrated.Impressively,the device at−0.78%strain and zero bias reveals a significantly enhanced photoresponse with a responsivity of 2.47 A W^(−1),a detectivity of 2.6×10^(11)Jones,and response times of 40/45μs,which are superior to the state-of-the-art self-powered flexible photodetectors.This work presents a valuable avenue to prepare tunable vdWs heterostructures for self-powered flexible photodetection,which performs well in flexible sensors.展开更多
Zinc Oxide(ZnO)has been extensively applied as electron transport material(ETM)in perovskite solar cells(PSCs)since the emergence of PSCs.However,some chemisorbed oxygen species on the surface of ZnO can cause the deg...Zinc Oxide(ZnO)has been extensively applied as electron transport material(ETM)in perovskite solar cells(PSCs)since the emergence of PSCs.However,some chemisorbed oxygen species on the surface of ZnO can cause the degradation of CH3NH3+(MA^(+))based perovskite.To avoid the destructive effect of ZnO,a facile solution strategy was proposed to produce a ZnS shell around the ZnO nanorods arrays(ZnO-NRs),i.e.ZnO@ZnS core-shell nanorods(ZnO-NRs@ZnS).The ZnO-NRs@ZnS cascade structure can not only facilitate carrier transport,but also enhance the stability of ZnO based PSCs.A power conversion efficiency(PCE)of 20.6%was finally yielded,which is the-state-of-the-art efficiency for PSCs with one-dimensional(1 D)ZnO electron transport materials(ETMs).Moreover,over 90%of the initial efficiency was retained for the unencapsulated device with ZnO-NRs@ZnS ETMs at 85℃for 500 h,demonstrating excellent stability.This work provides a simple and efficient avenue to simultaneously enhance the photovoltaic(PV)performance and stability of 1 D ZnO nanostructure-based PSCs.展开更多
The strong anisotropic electrical properties of one-dimensional(1 D) nanostructure semiconductors,especially the anisotropic carrier transport, have a negative and significant influence on the performance of solar cel...The strong anisotropic electrical properties of one-dimensional(1 D) nanostructure semiconductors,especially the anisotropic carrier transport, have a negative and significant influence on the performance of solar cells if the nanostructures have random orientation. Considering the advantages of nanorod solar cells in carrier transport, we have achieved growth of vertically aligned Sb_(2)Se_(3) nanorod array with highly(hk1) orientation on Cd S substrate, and constructed superstrate nanorod solar cells for the first time. The Sb_(2)Se_(3) nanorod array solar cells exhibit the more efficient and long-range carrier transport in vertical direction. Furthermore, in order to suppress interface recombination, a CuInSe_(2) quantum dots(QDs) sensitizer has been applied to fill the volume between the nanorods completely, thus forming an interpenetrating nanocomposite structure. The CuInSe_(2) QDs can harvest additional light by absorption of visible light and contribute photocurrent. Meantime, the QDs function as a hole transport material and thus reduce the dependence of lateral transport. Consequently, the interpenetrating nanocomposite CuInSe_(2) / Sb_(2)Se_(3) solar cells display a power conversion efficiency of 7.54% with significant enhancements in the short-circuit current density and open-circuit voltage over pure Sb_(2)Se_(3) nanorod cells. This is the highest efficiency for superstrate solar cells based on Sb_(2)Se_(3) nanorod arrays.展开更多
基金financially supported by the National Natural Science Foundation of China(21972068,22072067,22232004)the High-level Talents Project of Jinling Institute of Technology(jit-b-202164)。
文摘Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.
基金the financial support from the National Natural Science Foundation of China(U1732126,11804166,51602161,51372119)the Natural Science Foundation of Jiangsu Province(BK20150860)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX180846,KYCX180869)。
文摘Organometallic halide perovskite materials make great achievements in optoelectronic fields,especially in solar cells,in which the organic cations contain amine components.However,the amine with NàH bonds is easily hydrolyzed with moisture in the air,weakening the perovskite materials stability.It is desirable to develop other non-amine stable perovskite materials.In this work,sulfur-based perovskite-like(CH_(3))_(3)SPbI_(3) nanorod arrays were fabricated by a solution-processed method,which can be indexed hexagonal crystal structure in the space group P63 mc.The binding force is exceptionally strong between the non-amine(CH_(3))_(3) S+and[PbI_(6)]_(4)-octahedral,leading to high stability of(CH_(3))_(3)SPbI_(3).The(CH_(3))_(3)SPbI_(3) nanorod arrays can keep the morphology and crystal structure in an ambient atmosphere over 60 days.In addition,the(CH_(3))_(3)SPbI_(3) nanorod arrays can offer direct charge transfer channels,which show excellent optoelectronic properties.The(CH_(3))_(3)SPbI_(3) nanorod arrays-based solar cells with VOx hole transfer layers achieved a power conversion efficiency of 2.07%with negligible hysteresis.And the(CH_(3))_(3)SPbI_(3) nanorod arrays were also effectively applied in photodetectors with interdigitated gold electrodes.This work demonstrates that sulfur-based perovskite-like(CH_(3))_(3)SPbI_(3) is a novel promising stable compound with great potential for practical optoelectronic applications.
基金supported by the National Natural Science Foundation of China(Nos.12175190 and U2241284)the National Key R&D Program of China(Nos.SQ2022YFB190165)+1 种基金the Natural Science Foundation of Fujian Province,China(No.2022J02006)the Special Funds for Central Government Guiding Shenzhen Development in Science and Technology,China(No.2021Szvup066).
文摘Betavoltaic cells(BCs)are promising self-generating power cells with long life and high power density.However,the low energy conversion efficiency(ECE)has limitations in practical engineering applications.Widebandgap semiconductors(WBGSs)with three-dimensional(3-D)nanostructures are ideal candidates for increasing the ECE of BCs.This paper proposes hydrothermally grown ZnO nanorod arrays(ZNRAs)for ^(63)Ni-powered BCs.A quantitative model was established for simulation using the parameter values of the dark characteristics,which were obtained from the experimental measurements for a simulated BC based on a Ni-incorporated ZNRAs structure.Monte Carlo(MC)modeling and simulation were conducted to obtain the values of the β energy deposited in ZNRAs with different nanorod spacings and heights.Through the simulation and optimization of the 3-D ZNRAs and 2-D ZnO bulk structures,the performance of the ^(63)Ni-powered BCs based on both structures was evaluated using a quantitative model.The BCs based on the 3-D ZNRAs structure and 2-D ZnO bulk structure achieved a maximum ECE of 10.1%and 4.69%,respectively,which indicates the significant superiority of 3-D nanostructured WBGSs in increasing the ECE of BCs.
基金supported by the National Key Research and Development Program of China(2019YFA0705400 and 2019YFD0901100)the National Natural Science Foundation of China(21991151,21925404,and 21775127)+1 种基金the“111”Project(B17027)Guangdong Basic and Applied Basic Research Foundation(2020A1515010510)。
文摘All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a direct Z-scheme photoelectrocatalytic electrode based on a WO_(3-x)nanowire-bridged TiO_(2)nanorod array heterojunction is constructed for overall water splitting,producing H_(2).The as-prepared WO_(3-x)/TiO_(2)nanorod array heterojunction shows photoelectrochemical(PEC)overall water splitting activity evolving both H_(2) and O_(2)under UV-vis light irradiation.An optimum PEC activity was achieved over a 1.67-WO_(3-x)/TiO_(2)photoelectrode yielding maximum H_(2) and O_(2)evolution rates roughly 11 times higher than that of pure TiO_(2)nanorods without any sacrificial agent or redox mediator.The role of oxygen vacancy in WO_(3-x)in affecting the H_(2) production rate was also comprehensively studied.The superior PEC activity of the WO_(3-x)/TiO_(2)electrode for overall water splitting can be ascribed to an efficient Z-scheme charge transfer pathway between the WO_(3-x)nanowires and TiO_(2)nanorods,the presence of oxygen vacancies in WO_(3-x),and a bias potential applied on the photoelectrode,resulting in effective spatial charge separation.This study provides a novel strategy for developing highly efficient PECs for overall water splitting.
基金Project supported by the SONY-SINANO Joint Project (Grant No. Y1AAQ11001)the Suzhou Solar Cell Research Project,China (Grant No. ZXJ0903)+1 种基金the International S & T Cooperation Projects (SINO-Japan)the Science Fund of the Ministry of Science and Technology of the People’s Republic of China (Grant No. 2010DFA22770)
文摘InGaN/GaN epilayers, which are grown on sapphire substrates by the metal-organic chemical-vapour deposition （MOCVD） method, are formed into nanorod arrays using inductively coupled plasma etching via self-assembled Ni nanomasks. The formation of nanorod arrays eliminates the tilt of the InGaN （0002） crystallographic plane with respect to its GaN bulk layer. Photoluminescence results show an apparent S-shaped dependence on temperature. The light extraction efficiency and intensity of photoluminescence emission at low temperature of less than 30 K for the nanorod arrays are enhanced by the large surface area, which increases the quenching effect because of the high density of surface states for the temperature above 30 K. Additionally, a red-shift for the InGaN/GaN nanorod arrays is observed due to the strain relaxation, which is confirmed by reciprocal space mapping measurements.
基金supported by the National Key Research and Development Program of China(No.2022YFB3604500,No.2022YFB3604501)the National Natural Science Foundation of China(No.52172141)the Technology Development Project of Shanxi-Zheda Institude of Advanced Materials and Chemical Engineering(No.2022SX-TD017).
文摘van der Waals(vdW)heterostructures constructed by lowdimensional(0D,1D,and 2D)materials are emerging as one of the most appealing systems in next-generation flexible photodetection.Currently,hand-stacked vdW-type photodetectors are not compatible with large-areaarray fabrication and show unimpressive performance in self-powered mode.Herein,vertical 1D GaN nanorods arrays(NRAs)/2D MoS_(2)/PEDOT:PSS in wafer scale have been proposed for self-powered flexible photodetectors arrays firstly.The as-integrated device without external bias under weak UV illumination exhibits a competitive responsivity of 1.47 A W^(−1)and a high detectivity of 1.2×10^(11)Jones,as well as a fast response speed of 54/71μs,thanks to the strong light absorption of GaN NRAs and the efficient photogenerated carrier separation in type-II heterojunction.Notably,the strain-tunable photodetection performances of device have been demonstrated.Impressively,the device at−0.78%strain and zero bias reveals a significantly enhanced photoresponse with a responsivity of 2.47 A W^(−1),a detectivity of 2.6×10^(11)Jones,and response times of 40/45μs,which are superior to the state-of-the-art self-powered flexible photodetectors.This work presents a valuable avenue to prepare tunable vdWs heterostructures for self-powered flexible photodetection,which performs well in flexible sensors.
基金support from the National Natural Science Foundation of China(Grant Nos.21773218)the key research and development projects of Sichuan province(Grant No.2017GZ0052)+2 种基金the talents of science and technology innovation in Sichuan province(Grant No.2018RZ0119)the China Postdoctoral Science Foundation(Grant No.2019 M653485)Anshan Hifichem Co.Ltd.
文摘Zinc Oxide(ZnO)has been extensively applied as electron transport material(ETM)in perovskite solar cells(PSCs)since the emergence of PSCs.However,some chemisorbed oxygen species on the surface of ZnO can cause the degradation of CH3NH3+(MA^(+))based perovskite.To avoid the destructive effect of ZnO,a facile solution strategy was proposed to produce a ZnS shell around the ZnO nanorods arrays(ZnO-NRs),i.e.ZnO@ZnS core-shell nanorods(ZnO-NRs@ZnS).The ZnO-NRs@ZnS cascade structure can not only facilitate carrier transport,but also enhance the stability of ZnO based PSCs.A power conversion efficiency(PCE)of 20.6%was finally yielded,which is the-state-of-the-art efficiency for PSCs with one-dimensional(1 D)ZnO electron transport materials(ETMs).Moreover,over 90%of the initial efficiency was retained for the unencapsulated device with ZnO-NRs@ZnS ETMs at 85℃for 500 h,demonstrating excellent stability.This work provides a simple and efficient avenue to simultaneously enhance the photovoltaic(PV)performance and stability of 1 D ZnO nanostructure-based PSCs.
基金financially supported by the National Key R&D Program of China (Grant No. 2019YFB1503400)the National Natural Science Foundation of China (Grant No. 61804064)the Natural Science Foundation of Guangdong Province (Grant No.2019A1515011616)。
文摘The strong anisotropic electrical properties of one-dimensional(1 D) nanostructure semiconductors,especially the anisotropic carrier transport, have a negative and significant influence on the performance of solar cells if the nanostructures have random orientation. Considering the advantages of nanorod solar cells in carrier transport, we have achieved growth of vertically aligned Sb_(2)Se_(3) nanorod array with highly(hk1) orientation on Cd S substrate, and constructed superstrate nanorod solar cells for the first time. The Sb_(2)Se_(3) nanorod array solar cells exhibit the more efficient and long-range carrier transport in vertical direction. Furthermore, in order to suppress interface recombination, a CuInSe_(2) quantum dots(QDs) sensitizer has been applied to fill the volume between the nanorods completely, thus forming an interpenetrating nanocomposite structure. The CuInSe_(2) QDs can harvest additional light by absorption of visible light and contribute photocurrent. Meantime, the QDs function as a hole transport material and thus reduce the dependence of lateral transport. Consequently, the interpenetrating nanocomposite CuInSe_(2) / Sb_(2)Se_(3) solar cells display a power conversion efficiency of 7.54% with significant enhancements in the short-circuit current density and open-circuit voltage over pure Sb_(2)Se_(3) nanorod cells. This is the highest efficiency for superstrate solar cells based on Sb_(2)Se_(3) nanorod arrays.
