Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable ...Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion.In this regard,meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally necessary.Herein,a coordination environment inheriting strategy is presented for designing low-coordination Ni^(2+)octahedra(L-Ni-8)atomic interface at a high concentration(4.6 at.%).Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode.To improve the efficiency of using the self-modification reaction environment at L-Ni-8,all of the structural features,including high atom economy,mass transfer,and electron transfer,are integrated together from atomic-scale to macro-scale.At high current density of 500 mA/cm2,the samples synthesized at gram-scale can deliver low hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)overpotentials of 262 and 348 mV,respectively.展开更多
基金supported by the National Natural Science Foundation of China(No.21676300)the Shandong Provincial Natural Science Foundation(No.ZR2018MB035)+3 种基金the Fundamental Research Funds for the Central Universities(Nos.19CX02008A and 16CX06007A)PetroChina Innovation Foundation(No.2019D-5007-0401)Taishan Scholars Program of Shandong Province(No.tsqn201909065)Tsinghua University Initiative Scientific Research Program.
文摘Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion.In this regard,meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally necessary.Herein,a coordination environment inheriting strategy is presented for designing low-coordination Ni^(2+)octahedra(L-Ni-8)atomic interface at a high concentration(4.6 at.%).Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode.To improve the efficiency of using the self-modification reaction environment at L-Ni-8,all of the structural features,including high atom economy,mass transfer,and electron transfer,are integrated together from atomic-scale to macro-scale.At high current density of 500 mA/cm2,the samples synthesized at gram-scale can deliver low hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)overpotentials of 262 and 348 mV,respectively.
