Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nano...Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.展开更多
Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then...Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then Ru3+was introduced for ion exchange,and the porous Ru-doped Co_(3)O_(4)/rGO(Ru-Co_(3)O_(4)/rGO)composite electrocatalyst was prepared by annealing.The phase structure,morphology,and valence state of the catalyst were analyzed by X-ray powder diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).In 1 mol·L^(-1)KOH,the oxygen evolution reaction(OER)performance of the catalyst was measured by linear sweep voltammetry,cyclic voltammetry,and chronoamperometry.The results show that the combination of Ru doping and rGO provides a fast channel for collaborative electron transfer.At the same time,rGO as a carbon carrier can improve the electrical conductivity of Ru-Co_(3)O_(4)particles,and the uniformly dispersed nanoparticles enable the reactants to diffuse freely on the catalyst.The results showed that the electrochemical performance of Ru-Co_(3)O_(4)/rGO was much better than that of Co_(3)O_(4)/rGO,and the overpotential of Ru-Co_(3)O_(4)/rGO was 363.5 mV at the current density of 50 mA·cm^(-2).展开更多
Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled elec...The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.展开更多
Through employing zeolitic imidazolate framework-67(ZIF-67)templates,the straightforward hydrother-mal and electrodeposition methods were applied to synthesize FeOOH@CoMoO_(4)heterostructure attached to the sur-face o...Through employing zeolitic imidazolate framework-67(ZIF-67)templates,the straightforward hydrother-mal and electrodeposition methods were applied to synthesize FeOOH@CoMoO_(4)heterostructure attached to the sur-face of nickel foam(NF).The specific structure of the as-prepared FeOOH@CoMoO_(4)/NF-400s provided pronounced porosity and extensive surface area,enhancing rapid electron transport and exposing abundant active sites to improve catalytic reactions.Furthermore,the introduction of FeOOH,which induces electron transfer from FeOOH to CoMoO_(4),confirms their strong electronic interaction,thereby leading to an accelerated surface catalytic reaction.Consequently,the constructed FeOOH@CoMoO_(4)/NF-400s heterostructure demonstrated exceptional oxygen evolu-tion reaction(OER)activity,requiring an overpotential of 199 mV to deliver the current density of 10 mA·cm^(-2),cou-pled with the superior Tafel slope value of 49.56 mV·dec^(-1)and outstanding stability over 20 h under the current densities of both 10 and 100 mA·cm^(-2).展开更多
Recovering valuable metals from spent lithium-ion batteries(LIBs)for high value-added application is beneficial for global energy cycling and environmental protection.In this work,we obtain the high-performance N-dope...Recovering valuable metals from spent lithium-ion batteries(LIBs)for high value-added application is beneficial for global energy cycling and environmental protection.In this work,we obtain the high-performance N-doped Ni-Co-Mn(N-NCM)electrocatalyst from waste LIBs,for robust oxygen evolution application.Lithium-rich solution and NCM oxides are effectively separated from ternary cathode materials by sulfation roasting and low-temperature water leaching approach,in which the recovery efficiency of Li metal reaches nearly 100%.By facile NH_(3)treatment,the incorporation of N into NCM significantly increases the ratio of low-valence state Co^(2+)and Mn^(2+),and the formed Mn-N bond benefits the surface catalytic kinetics.Meanwhile,the N doping induces lattice expansion of the NCM,triggering tensile stress to favor the adsorption of the reactant.Thus,the optimized N-NCM electrocatalyst exhibits the superior overpotentials of 256 and 453 mV to achieve the current density of 10 and 100 mA/cm^(2),respectively,with a low Tafel slope of 37.3 mV/dec.This work provides a fresh avenue for recycling spent LIBs in the future to achieve sustainable development.展开更多
A new anodic material of ternary Pb-0.8%Ag-(0-5.0%)Bi alloy for zinc electrowinning was obtained by doping Bi.The anodic oxygen evolution potential,corrosion rate,surface products after polarization,and microstructure...A new anodic material of ternary Pb-0.8%Ag-(0-5.0%)Bi alloy for zinc electrowinning was obtained by doping Bi.The anodic oxygen evolution potential,corrosion rate,surface products after polarization,and microstructures before and after polarization were studied and compared with those of Pb-0.8%Ag anode used in industry.The results show the anodic overpotential decreases with the increase of Bi content in the alloys.When the content of Bi is 1.0%(mass fraction),the anodic overpotential is 40-50 mV lower than that of Pb-0.8%Ag anode.While the corrosion rate decreases and then increases with the increase of Bi content.The Pb-0.8%Ag-0.1%Bi anode has the lowest corrosion rate(0.090 6 mg/(h·cm2).Doping Bi influences the structure of the anodic layer,but does not change the phase.The Pb-0.8%Ag-1.0%Bi anode layer is of a more fine-grained structure compared with Pb-0.8%Ag anode.展开更多
Developing efficient,durable,and precious metal-free electrocatalysts is currently a huge challenge.In this article,through a simple one-step high-temperature pyrolysis method,by incorporating various non-metallic ele...Developing efficient,durable,and precious metal-free electrocatalysts is currently a huge challenge.In this article,through a simple one-step high-temperature pyrolysis method,by incorporating various non-metallic element atoms,we prepared four different NiX(X=Cl_(2),(CH_(3)COO)_(2),(NO_(3))2,SO_(4))@CNT catalysts.Additionally,by adjusting the temperature,these four materials were expanded into twelve catalyst materials for comparative optimization of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activity.Ultimately,Ni(NO_(3))2@CNT-900 typically exhibits superior OER and HER activity.In 1 mol/L KOH solution with a current density of 10 mA/cm^(2),the overpotentials of HER and OER of Ni(NO_(3))2@CNT-900 are only 145 mV and 300 mV,respectively.Furthermore,the Ni(NO_(3))2@CNT-900 shows excellent durability in both HER and OER.展开更多
Heterojunction catalysts composed of transition metal sulfides exhibited excellent potentials in electrocatalytic water splitting.Herein,we have designed a FeS/Co_(3)S_(4) heterojunction catalyst for hydrogen evolutio...Heterojunction catalysts composed of transition metal sulfides exhibited excellent potentials in electrocatalytic water splitting.Herein,we have designed a FeS/Co_(3)S_(4) heterojunction catalyst for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline water/seawater solution.Three-dimensional nanoarrays were grown on nickel foam,and the successful synthesis of heterojunction endowed excellent activity to the catalyst.In alkaline water/seawater solution,the low overpotentials(at current density of 10 mA/cm^(2))of HER were 120.3 and 135.6 mV and the low overpotentials of OER were 212 and 232 mV,respectively.This work provided an effective method for highly-efficiently electrocatalytic splitting of water via fabrication of heterojunction.展开更多
Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer...Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to accelerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)_(2)nanosheets.Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER.Specifically,Co_(n)Ir_(1)/Ni(OH)_(2)required an overpotential of 255 mV at a current density of 10 mA·cm^(−2),which was 60 mV and 67 mV lower than those of Co_(n)/Ni(OH)_(2)and Ir1/Ni(OH)_(2),respectively.The turnover frequency of Co_(n)Ir_(1)/Ni(OH)_(2)was 0.49 s^(−1),which was 4.9 times greater than that of Co_(n)/Ni(OH)_(2)at an overpotential of 300 mV.展开更多
TiO2/Nb2O5 photocatalyst loaded with WO3 （WO3-TiO2/Nb2O5） was prepared by a modified hydrolysis process, and characterized by X-ray diffractometry, transmission electron microscopy, Raman spectra and UV-Vis diffuse ...TiO2/Nb2O5 photocatalyst loaded with WO3 （WO3-TiO2/Nb2O5） was prepared by a modified hydrolysis process, and characterized by X-ray diffractometry, transmission electron microscopy, Raman spectra and UV-Vis diffuse refraction spectroscopy. The photocatalytic activity of WO3-TiO2/Nb2O5 was investigated by employing splitting of water for O2 evolution. The results indicate that WO3 loading can pronouncedly improve the photocatalytic activity of TiOjNb2O5 by using Fe^3＋ as an electron acceptor under UV irradiation. The optimum molar fraction of the loaded WO3 is 2%, and the largest speed of O2 evolution for 2% WO3-TiO2/Nb2O5 catalyst is 151.8 μmol/（L·h）.展开更多
Non-precious electro catalysts with high-efficiency, cheapness and stablility are of great significance to replace noble metal electro catalysts in the hydrogen evolution reaction(HER) and oxygen evolution reaction(OE...Non-precious electro catalysts with high-efficiency, cheapness and stablility are of great significance to replace noble metal electro catalysts in the hydrogen evolution reaction(HER) and oxygen evolution reaction(OER). In this work, triangular Cu@CuO nanorods on Cu nanosheets were fabricated by a novel in-situ oxidation approach using Cu nanosheets as self-template and conductive nano-substrate in an aqueous solution of NaOH/H2O2, and then by lowtemperature phosphorization treatments. The experimental results show that the phosphating temperature has a significant effect on the morphology, composition and number of active sites of Cu@Cu_(3)P nanorods. The Cu@Cu_(3)P-280 electrode exhibits a good HER catalytic activity of achieving a current density of 10 mA/cm^(2) at 252 mV in acid electrolyte. After catalysis for 14 h, the current density can still reach 72% of the initial value. Moreover, the Cu@Cu_(3)P-280 electrode also shows an excellent OER catalytic activity in basic electrolyte, reaching a current density of 10 mA/cm^(2) at the overpotential value of 200 mV. After catalysis for 12 h, the current density remained more than 93% of the initial value. This work provides a theoretical basis for the directional design and preparation of sustainable, low-cost, bifunctional electrocatalytic materials.展开更多
Exploiting highly active and non-noble metal bifunctional catalysts at large current density is significant for the advancement of water electrolysis.In this work,CeO_(2)electronically structure modulated FeNi bimetal...Exploiting highly active and non-noble metal bifunctional catalysts at large current density is significant for the advancement of water electrolysis.In this work,CeO_(2)electronically structure modulated FeNi bimetallic composite porous nanosheets in-situ grown on nickel foam(NiFe_(2)O_(4)-Fe_(24)N_(10)-CeO_(2)/NF)is synthesized.Electrochemical experiments show that the NiFe_(2)O_(4)-Fe_(24)N_(10)-CeO_(2)/NF exhibited the outstanding activities toward both oxygen and hydrogen evolution reactions(OER and HER)(η1000=352 mV andη1000=429 mV,respectively).When assembled into a two-electrode system for overall water splitting(OWS),it only needs a low cell voltage of 1.81 V to drive 100 mA·cm^(-2).And it can operate stably at±500 mA·cm^(-2)over 30 h toward OER,HER and OWS without significant activity changes.The reason could be assigned to the electronic modulating of CeO_(2)on FeNi composite,which can boost the intrinsic activity and optimize the adsorption of reaction intermediates.Moreover,the porous nanosheets insitu grown on NF could enhance the contact of active site with electrolyte and facilitate the gas release,thus improving its chemical and mechanical stabilities.This study highlights a novel approach to design bifunctional non-noble metal catalysts for water splitting at large current density.展开更多
The unavailability of high-performance and cost-effective electrocatalysts has impeded the large-scale deployment of alkaline water electrolyzers.Professor Zidong Wei's group has focused on resolving critical chal...The unavailability of high-performance and cost-effective electrocatalysts has impeded the large-scale deployment of alkaline water electrolyzers.Professor Zidong Wei's group has focused on resolving critical challenges in industrial alkaline electrolysis,particularly elucidating hydrogen and oxygen evolution reaction(HER/OER)mechanisms while addressing the persistent activity-stability trade-off.This review summarizes their decade-long progress in developing advanced electrodes,analyzing the origins of sluggish alkaline HER kinetics and OER stability limitations.Professor Wei proposes a unifying"12345 Principle"as an optimization framework.For HER electrocatalysts,they have identified that metal/metal oxide interfaces create synergistic"chimney effect"and"local electric field enhancement effect",enhancing selective intermediate adsorption,interfacial water enrichment/reorientation,and mass transport under industrial high-polarization conditions.Regarding OER,innovative strategies,including dual-ligand synergistic modulation,lattice oxygen suppression,and self-repairing surface construction,are demonstrated to balance oxygen species adsorption,optimize spin states,and dynamically reinforce metal-oxygen bonds for concurrent activity-stability enhancement.The review concludes by addressing remaining challenges in long-term industrial durability and suggesting future research priorities.展开更多
文摘Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.
文摘Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then Ru3+was introduced for ion exchange,and the porous Ru-doped Co_(3)O_(4)/rGO(Ru-Co_(3)O_(4)/rGO)composite electrocatalyst was prepared by annealing.The phase structure,morphology,and valence state of the catalyst were analyzed by X-ray powder diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).In 1 mol·L^(-1)KOH,the oxygen evolution reaction(OER)performance of the catalyst was measured by linear sweep voltammetry,cyclic voltammetry,and chronoamperometry.The results show that the combination of Ru doping and rGO provides a fast channel for collaborative electron transfer.At the same time,rGO as a carbon carrier can improve the electrical conductivity of Ru-Co_(3)O_(4)particles,and the uniformly dispersed nanoparticles enable the reactants to diffuse freely on the catalyst.The results showed that the electrochemical performance of Ru-Co_(3)O_(4)/rGO was much better than that of Co_(3)O_(4)/rGO,and the overpotential of Ru-Co_(3)O_(4)/rGO was 363.5 mV at the current density of 50 mA·cm^(-2).
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
基金supported by the National Natural Science Foundation of China(22209040,22202063).
文摘The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.
文摘Through employing zeolitic imidazolate framework-67(ZIF-67)templates,the straightforward hydrother-mal and electrodeposition methods were applied to synthesize FeOOH@CoMoO_(4)heterostructure attached to the sur-face of nickel foam(NF).The specific structure of the as-prepared FeOOH@CoMoO_(4)/NF-400s provided pronounced porosity and extensive surface area,enhancing rapid electron transport and exposing abundant active sites to improve catalytic reactions.Furthermore,the introduction of FeOOH,which induces electron transfer from FeOOH to CoMoO_(4),confirms their strong electronic interaction,thereby leading to an accelerated surface catalytic reaction.Consequently,the constructed FeOOH@CoMoO_(4)/NF-400s heterostructure demonstrated exceptional oxygen evolu-tion reaction(OER)activity,requiring an overpotential of 199 mV to deliver the current density of 10 mA·cm^(-2),cou-pled with the superior Tafel slope value of 49.56 mV·dec^(-1)and outstanding stability over 20 h under the current densities of both 10 and 100 mA·cm^(-2).
基金Project(2022YFC3900804)supported by the National Key Research and Development Program,ChinaProjects(2021JJ10058,2022JJ10074)supported by the Natural Science Foundation of Hunan Province of China。
文摘Recovering valuable metals from spent lithium-ion batteries(LIBs)for high value-added application is beneficial for global energy cycling and environmental protection.In this work,we obtain the high-performance N-doped Ni-Co-Mn(N-NCM)electrocatalyst from waste LIBs,for robust oxygen evolution application.Lithium-rich solution and NCM oxides are effectively separated from ternary cathode materials by sulfation roasting and low-temperature water leaching approach,in which the recovery efficiency of Li metal reaches nearly 100%.By facile NH_(3)treatment,the incorporation of N into NCM significantly increases the ratio of low-valence state Co^(2+)and Mn^(2+),and the formed Mn-N bond benefits the surface catalytic kinetics.Meanwhile,the N doping induces lattice expansion of the NCM,triggering tensile stress to favor the adsorption of the reactant.Thus,the optimized N-NCM electrocatalyst exhibits the superior overpotentials of 256 and 453 mV to achieve the current density of 10 and 100 mA/cm^(2),respectively,with a low Tafel slope of 37.3 mV/dec.This work provides a fresh avenue for recycling spent LIBs in the future to achieve sustainable development.
基金Project(2007SK2009)supported by the Science and Technology Research Project of Hunan Province,China
文摘A new anodic material of ternary Pb-0.8%Ag-(0-5.0%)Bi alloy for zinc electrowinning was obtained by doping Bi.The anodic oxygen evolution potential,corrosion rate,surface products after polarization,and microstructures before and after polarization were studied and compared with those of Pb-0.8%Ag anode used in industry.The results show the anodic overpotential decreases with the increase of Bi content in the alloys.When the content of Bi is 1.0%(mass fraction),the anodic overpotential is 40-50 mV lower than that of Pb-0.8%Ag anode.While the corrosion rate decreases and then increases with the increase of Bi content.The Pb-0.8%Ag-0.1%Bi anode has the lowest corrosion rate(0.090 6 mg/(h·cm2).Doping Bi influences the structure of the anodic layer,but does not change the phase.The Pb-0.8%Ag-1.0%Bi anode layer is of a more fine-grained structure compared with Pb-0.8%Ag anode.
基金Project(145209113)supported by the Basic Research Expenses of Department of Education of Heilongjiang Province,China。
文摘Developing efficient,durable,and precious metal-free electrocatalysts is currently a huge challenge.In this article,through a simple one-step high-temperature pyrolysis method,by incorporating various non-metallic element atoms,we prepared four different NiX(X=Cl_(2),(CH_(3)COO)_(2),(NO_(3))2,SO_(4))@CNT catalysts.Additionally,by adjusting the temperature,these four materials were expanded into twelve catalyst materials for comparative optimization of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activity.Ultimately,Ni(NO_(3))2@CNT-900 typically exhibits superior OER and HER activity.In 1 mol/L KOH solution with a current density of 10 mA/cm^(2),the overpotentials of HER and OER of Ni(NO_(3))2@CNT-900 are only 145 mV and 300 mV,respectively.Furthermore,the Ni(NO_(3))2@CNT-900 shows excellent durability in both HER and OER.
基金supported by the Dean/Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2023K001)Taishan Scholars Foundation of Shandong province(TSQN201909058).
文摘Heterojunction catalysts composed of transition metal sulfides exhibited excellent potentials in electrocatalytic water splitting.Herein,we have designed a FeS/Co_(3)S_(4) heterojunction catalyst for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline water/seawater solution.Three-dimensional nanoarrays were grown on nickel foam,and the successful synthesis of heterojunction endowed excellent activity to the catalyst.In alkaline water/seawater solution,the low overpotentials(at current density of 10 mA/cm^(2))of HER were 120.3 and 135.6 mV and the low overpotentials of OER were 212 and 232 mV,respectively.This work provided an effective method for highly-efficiently electrocatalytic splitting of water via fabrication of heterojunction.
基金supported by the National Key Research and Development Program of China(2021YFA1500500,2019-YFA0405600)the CAS Project for Young Scientists in Basic Research(YSBR-051)+6 种基金the National Science Fund for Distinguished Young Scholars(21925204)the National Natural Science Foundation of China(22202192,U19A2015,22221003,22250007,22163002)the Collaborative Innovation Program of Hefei Science Center,CAS(2022HSCCIP004)the International Partnership,the DNL Cooperation Fund,CAS(DNL202003)the USTC Research Funds of the Double First-Class Initiative(YD9990002016,YD999000-2014)the Program of Chinese Academy of Sciences(123GJHZ2022101GC)the Fundamental Research Funds for the Central Universities(WK9990000095,WK999000-0124).
文摘Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to accelerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)_(2)nanosheets.Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER.Specifically,Co_(n)Ir_(1)/Ni(OH)_(2)required an overpotential of 255 mV at a current density of 10 mA·cm^(−2),which was 60 mV and 67 mV lower than those of Co_(n)/Ni(OH)_(2)and Ir1/Ni(OH)_(2),respectively.The turnover frequency of Co_(n)Ir_(1)/Ni(OH)_(2)was 0.49 s^(−1),which was 4.9 times greater than that of Co_(n)/Ni(OH)_(2)at an overpotential of 300 mV.
基金Project(2002AA327140) supported by National High-Tech Research and Development Program of China
文摘TiO2/Nb2O5 photocatalyst loaded with WO3 （WO3-TiO2/Nb2O5） was prepared by a modified hydrolysis process, and characterized by X-ray diffractometry, transmission electron microscopy, Raman spectra and UV-Vis diffuse refraction spectroscopy. The photocatalytic activity of WO3-TiO2/Nb2O5 was investigated by employing splitting of water for O2 evolution. The results indicate that WO3 loading can pronouncedly improve the photocatalytic activity of TiOjNb2O5 by using Fe^3＋ as an electron acceptor under UV irradiation. The optimum molar fraction of the loaded WO3 is 2%, and the largest speed of O2 evolution for 2% WO3-TiO2/Nb2O5 catalyst is 151.8 μmol/（L·h）.
基金Project(21905232) supported by the National Natural Science Foundation of China。
文摘Non-precious electro catalysts with high-efficiency, cheapness and stablility are of great significance to replace noble metal electro catalysts in the hydrogen evolution reaction(HER) and oxygen evolution reaction(OER). In this work, triangular Cu@CuO nanorods on Cu nanosheets were fabricated by a novel in-situ oxidation approach using Cu nanosheets as self-template and conductive nano-substrate in an aqueous solution of NaOH/H2O2, and then by lowtemperature phosphorization treatments. The experimental results show that the phosphating temperature has a significant effect on the morphology, composition and number of active sites of Cu@Cu_(3)P nanorods. The Cu@Cu_(3)P-280 electrode exhibits a good HER catalytic activity of achieving a current density of 10 mA/cm^(2) at 252 mV in acid electrolyte. After catalysis for 14 h, the current density can still reach 72% of the initial value. Moreover, the Cu@Cu_(3)P-280 electrode also shows an excellent OER catalytic activity in basic electrolyte, reaching a current density of 10 mA/cm^(2) at the overpotential value of 200 mV. After catalysis for 12 h, the current density remained more than 93% of the initial value. This work provides a theoretical basis for the directional design and preparation of sustainable, low-cost, bifunctional electrocatalytic materials.
基金supported by the National Natural Science Foundation of China(22162004)the Natural Science Foundation of Guangxi Province(2022JJD120011).
文摘Exploiting highly active and non-noble metal bifunctional catalysts at large current density is significant for the advancement of water electrolysis.In this work,CeO_(2)electronically structure modulated FeNi bimetallic composite porous nanosheets in-situ grown on nickel foam(NiFe_(2)O_(4)-Fe_(24)N_(10)-CeO_(2)/NF)is synthesized.Electrochemical experiments show that the NiFe_(2)O_(4)-Fe_(24)N_(10)-CeO_(2)/NF exhibited the outstanding activities toward both oxygen and hydrogen evolution reactions(OER and HER)(η1000=352 mV andη1000=429 mV,respectively).When assembled into a two-electrode system for overall water splitting(OWS),it only needs a low cell voltage of 1.81 V to drive 100 mA·cm^(-2).And it can operate stably at±500 mA·cm^(-2)over 30 h toward OER,HER and OWS without significant activity changes.The reason could be assigned to the electronic modulating of CeO_(2)on FeNi composite,which can boost the intrinsic activity and optimize the adsorption of reaction intermediates.Moreover,the porous nanosheets insitu grown on NF could enhance the contact of active site with electrolyte and facilitate the gas release,thus improving its chemical and mechanical stabilities.This study highlights a novel approach to design bifunctional non-noble metal catalysts for water splitting at large current density.
基金the National Key R&D Program of China(2021YFB4000300)National Natural Science Foundation of China(21822803,22408030,22072009,91534205,51072239)National Program on Key Basic Research Project(973 Program,2012CB720303).
文摘The unavailability of high-performance and cost-effective electrocatalysts has impeded the large-scale deployment of alkaline water electrolyzers.Professor Zidong Wei's group has focused on resolving critical challenges in industrial alkaline electrolysis,particularly elucidating hydrogen and oxygen evolution reaction(HER/OER)mechanisms while addressing the persistent activity-stability trade-off.This review summarizes their decade-long progress in developing advanced electrodes,analyzing the origins of sluggish alkaline HER kinetics and OER stability limitations.Professor Wei proposes a unifying"12345 Principle"as an optimization framework.For HER electrocatalysts,they have identified that metal/metal oxide interfaces create synergistic"chimney effect"and"local electric field enhancement effect",enhancing selective intermediate adsorption,interfacial water enrichment/reorientation,and mass transport under industrial high-polarization conditions.Regarding OER,innovative strategies,including dual-ligand synergistic modulation,lattice oxygen suppression,and self-repairing surface construction,are demonstrated to balance oxygen species adsorption,optimize spin states,and dynamically reinforce metal-oxygen bonds for concurrent activity-stability enhancement.The review concludes by addressing remaining challenges in long-term industrial durability and suggesting future research priorities.
