Surface strain engineering is a promising strategy to design various electrocatalysts for sustainable energy storage and conversion.However,achieving the multifunctional activity of the catalyst via the adjustment of ...Surface strain engineering is a promising strategy to design various electrocatalysts for sustainable energy storage and conversion.However,achieving the multifunctional activity of the catalyst via the adjustment of strain engineering remains a major challenge.Herein,an excellent trifunctional electrocatalyst(Ru/RuO_(2)@NCS)is prepared by anchoring lattice mismatch strained core/shell Ru/RuO_(2)nanocrystals on nitrogen-doped carbon nanosheets.Core/shell Ru/RuO_(2)nanocrystals with~5 atomic layers of RuO_(2)shells eliminate the ligand effect and produce~2%of the surface compressive strain,which can boost the trifunctional activity(oxygen evolution reaction[OER],oxygen reduction reaction[ORR],and hydrogen evolution reaction[HER])of the catalyst.When equipped in rechargeable Zn-air batteries,the Ru/RuO_(2)@NCS endows them with high power(137.1 mW cm^(2))and energy(714.9 Wh kg_(Zn)^(-1))density and excellent cycle stability.Moreover,the as-fabricated Zn-air batteries can drive a water splitting electrolyzer assembled with Ru/RuO_(2)@NCS and achieve a current density of 10 mA cm^(2)only requires a low potential~1.51 V.Density functional theory calculations reveal that the compressive strained RuO_(2)could reduce the reaction barrier and improve the binding of rate-determining intermediates(*OH,*O,*OOH,and*H),leading to the enhanced catalytic activity and stability.This work can provide a novel avenue for the rational design of multifunctional catalysts in future clean energy fields.展开更多
Main observation and conclusion Perovskites(Ba_(0.5)Sr_(0.5))_(1-x)Co_(0.8)Fe_(0.2)O_(3-δ)(x=0.02,0.05,0.1 denoted as BSCF-0.98,BSCF-0.95,BSCF-0.9,respectively)with A-site cation defects are synthesized by simple and...Main observation and conclusion Perovskites(Ba_(0.5)Sr_(0.5))_(1-x)Co_(0.8)Fe_(0.2)O_(3-δ)(x=0.02,0.05,0.1 denoted as BSCF-0.98,BSCF-0.95,BSCF-0.9,respectively)with A-site cation defects are synthesized by simple and efficient sol-gel method and are proved to have better OER catalytic effect than the well-known(Ba_(0.5)Sr_(0.5))_(1-x)Co_(0.8)Fe_(0.2)O_(3-δ)(BSCF)oxides.BSCF-0.95 exhibits the best OER catalytic activity in the series perovskite.The current density of BSCF-0.95 is about 56%higher than that of BSCF oxide at a potential of 1.7 V.The experimental studies have shown that compared with BSCF,BSCF-0.95 oxide has a larger electrochemical surface area(ECSA),a higher content of O_(2)^(2–)species related to surface oxygen vacancies,and faster charge transfer rate,which may be the factors for the enhancement of OER activity.The theoretical calculation results prove that the center positions of the O 2p-band of perovskite with A-site cation defects are closer to the Fermi level than BSCF oxide,which agrees with the OER performance trend of the material.展开更多
基金the Key projects of intergovernmental international cooperation in key R&D programs of the Ministry of science and technology of China,Grant/Award Number:2021YFE0115800National Science Funding Committee of China,Grant/Award Number:U20A20250+1 种基金China Postdoctoral Science Foundation,Grant/Award Number:2020M673630XBScience and Technology Committee of Shaanxi Province,Grant/Award Number:2020JZ-42。
文摘Surface strain engineering is a promising strategy to design various electrocatalysts for sustainable energy storage and conversion.However,achieving the multifunctional activity of the catalyst via the adjustment of strain engineering remains a major challenge.Herein,an excellent trifunctional electrocatalyst(Ru/RuO_(2)@NCS)is prepared by anchoring lattice mismatch strained core/shell Ru/RuO_(2)nanocrystals on nitrogen-doped carbon nanosheets.Core/shell Ru/RuO_(2)nanocrystals with~5 atomic layers of RuO_(2)shells eliminate the ligand effect and produce~2%of the surface compressive strain,which can boost the trifunctional activity(oxygen evolution reaction[OER],oxygen reduction reaction[ORR],and hydrogen evolution reaction[HER])of the catalyst.When equipped in rechargeable Zn-air batteries,the Ru/RuO_(2)@NCS endows them with high power(137.1 mW cm^(2))and energy(714.9 Wh kg_(Zn)^(-1))density and excellent cycle stability.Moreover,the as-fabricated Zn-air batteries can drive a water splitting electrolyzer assembled with Ru/RuO_(2)@NCS and achieve a current density of 10 mA cm^(2)only requires a low potential~1.51 V.Density functional theory calculations reveal that the compressive strained RuO_(2)could reduce the reaction barrier and improve the binding of rate-determining intermediates(*OH,*O,*OOH,and*H),leading to the enhanced catalytic activity and stability.This work can provide a novel avenue for the rational design of multifunctional catalysts in future clean energy fields.
基金supported by the National Natural Science Foundation of China(No.21671182)the Fundamental Research Funds for the Central Universities(WK3430000005))The calculations were performed on the supercomputing center of the University of Science and Technology of China(USTC-SCC).
文摘Main observation and conclusion Perovskites(Ba_(0.5)Sr_(0.5))_(1-x)Co_(0.8)Fe_(0.2)O_(3-δ)(x=0.02,0.05,0.1 denoted as BSCF-0.98,BSCF-0.95,BSCF-0.9,respectively)with A-site cation defects are synthesized by simple and efficient sol-gel method and are proved to have better OER catalytic effect than the well-known(Ba_(0.5)Sr_(0.5))_(1-x)Co_(0.8)Fe_(0.2)O_(3-δ)(BSCF)oxides.BSCF-0.95 exhibits the best OER catalytic activity in the series perovskite.The current density of BSCF-0.95 is about 56%higher than that of BSCF oxide at a potential of 1.7 V.The experimental studies have shown that compared with BSCF,BSCF-0.95 oxide has a larger electrochemical surface area(ECSA),a higher content of O_(2)^(2–)species related to surface oxygen vacancies,and faster charge transfer rate,which may be the factors for the enhancement of OER activity.The theoretical calculation results prove that the center positions of the O 2p-band of perovskite with A-site cation defects are closer to the Fermi level than BSCF oxide,which agrees with the OER performance trend of the material.
