Currently,global warming and energy problems become more and more serious with the development of economy and the continuous consumption of fossil fuel,which are due to the release of greenhouse gas in the process of ...Currently,global warming and energy problems become more and more serious with the development of economy and the continuous consumption of fossil fuel,which are due to the release of greenhouse gas in the process of fossil fuel combustion and industrial manufacturing.展开更多
Electrochemical nitrate reduction reaction(NO_(3)−RR)is an ideal route to produce ammonia(NH_(3))under ambient conditions.Although a markedly improved NH3 production rate has been achieved on the NO_(3)−RR compared wi...Electrochemical nitrate reduction reaction(NO_(3)−RR)is an ideal route to produce ammonia(NH_(3))under ambient conditions.Although a markedly improved NH3 production rate has been achieved on the NO_(3)−RR compared with the nitrogen reduction reaction(NRR),the NH_(3) production rate of NO_(3)−RR is still well below the industrial Haber-Bosch route due to the lack of robust electrocatalysts for yielding high current densitieswith concurrently good suppression of hydrogen evolution reaction(HER).Herein,we describe an in situ electrochemical strategy for the synthesis of hollow carbon-coated Cu nanoparticles(NPs)(HSCu@C)with abundant grain boundaries(HSCu-AGB@C)for highly efficient NO_(3)−RR in both alkaline and neutral media.Impressively,in alkaline media,the HSCu-AGB@C can achieve a maximum NH3 Faradaic efficiency of 94.2% with an ultrahigh NH_(3) rate of 487.8 mmol g^(−1) cat h^(−1) at−0.2 V versus a reversible hydrogen electrode,more than 2.4-fold of the rate obtained in the Haber-Bosch.Both theoretic computations and experimental results uncover that the grain boundaries play the key to improve the NO_(3)−RR performance.Herein,the industrial-scale NH_(3) production ratemay open exciting opportunities for the practical electrosynthesis NH_(3) under ambient conditions.展开更多
Self-standing porous WP2 nanosheet arrays on carbon fiber cloth （WP2 NSs/CC） were synthesized and used as a 3D flexible hydrogen evolution electrode. Because of its 3D porous nanoarray structure, the WP2 NSs/CC exhi...Self-standing porous WP2 nanosheet arrays on carbon fiber cloth （WP2 NSs/CC） were synthesized and used as a 3D flexible hydrogen evolution electrode. Because of its 3D porous nanoarray structure, the WP2 NSs/CC exhibits a remarkable catalytic activity and a high stability. By using the experimental measurements and first-principle calculations, the underlying reasons for the excellent catalytic activity were further explored. Our work makes the present WPz NSs as a promising electrocatalyst for hydrogen evolution and provides a way to design and fabricate efficient hydrogen evolution electrodes through 3D porous nano-arrays architecture.展开更多
基金supported by the National Natural Science Foundation(NNSF)of China(21975162 and 21574084)the Shenzhen Government’s Plan of Science and Technology(JCYJ20170818091657056)。
文摘Currently,global warming and energy problems become more and more serious with the development of economy and the continuous consumption of fossil fuel,which are due to the release of greenhouse gas in the process of fossil fuel combustion and industrial manufacturing.
基金the National Natural Science Foundation(NNSF)of China(nos.21975162 and 51902208)Shenzhen Government’s Plan of Science and Technology(nos.JCYJ20200109105803806 and JCYJ20190808142219049).
文摘Electrochemical nitrate reduction reaction(NO_(3)−RR)is an ideal route to produce ammonia(NH_(3))under ambient conditions.Although a markedly improved NH3 production rate has been achieved on the NO_(3)−RR compared with the nitrogen reduction reaction(NRR),the NH_(3) production rate of NO_(3)−RR is still well below the industrial Haber-Bosch route due to the lack of robust electrocatalysts for yielding high current densitieswith concurrently good suppression of hydrogen evolution reaction(HER).Herein,we describe an in situ electrochemical strategy for the synthesis of hollow carbon-coated Cu nanoparticles(NPs)(HSCu@C)with abundant grain boundaries(HSCu-AGB@C)for highly efficient NO_(3)−RR in both alkaline and neutral media.Impressively,in alkaline media,the HSCu-AGB@C can achieve a maximum NH3 Faradaic efficiency of 94.2% with an ultrahigh NH_(3) rate of 487.8 mmol g^(−1) cat h^(−1) at−0.2 V versus a reversible hydrogen electrode,more than 2.4-fold of the rate obtained in the Haber-Bosch.Both theoretic computations and experimental results uncover that the grain boundaries play the key to improve the NO_(3)−RR performance.Herein,the industrial-scale NH_(3) production ratemay open exciting opportunities for the practical electrosynthesis NH_(3) under ambient conditions.
文摘Self-standing porous WP2 nanosheet arrays on carbon fiber cloth （WP2 NSs/CC） were synthesized and used as a 3D flexible hydrogen evolution electrode. Because of its 3D porous nanoarray structure, the WP2 NSs/CC exhibits a remarkable catalytic activity and a high stability. By using the experimental measurements and first-principle calculations, the underlying reasons for the excellent catalytic activity were further explored. Our work makes the present WPz NSs as a promising electrocatalyst for hydrogen evolution and provides a way to design and fabricate efficient hydrogen evolution electrodes through 3D porous nano-arrays architecture.
