Regulating the interfacial charge transfer and constructing symmetry-breaking sites for the enhanced N_(2) electroreduction activity  

作　　者：Xiaoxue Zhang Yuehan Cao Zhen-Feng Huang Shishi Zhang Chengguang Liu Lun Pan Chengxiang Shi Xiangwen Zhang Ying Zhou Guidong Yang Ji-Jun Zou 

机构地区：[1]Key Laboratory for Green Chemical Technology of the Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin,China [2]Collaborative Innovative Center of Chemical Science and Engineering(Tianjin),Tianjin,China [3]Zhejiang Institute of Tianjin University,Ningbo,Zhejiang,China [4]State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation,School of New Energy and Materials,Institute of Carbon Neutrality,Southwest Petroleum University,Chengdu,Sichuan,China [5]XJTU-Oxford International Joint Laboratory for Catalysis,School of Chemical Engineering and Technology,Xi'an Jiaotong University,Xi'an,Shaanxi,China

出　　处：《Carbon Energy》2023年第2期193-200,共8页碳能源（英文）

基　　金：National Key R&D Program of China,Grant/Award Number:2020YFA0710000;National Natural Science Foundation of China,Grant/Award Numbers:22008170,21978200,22161142002,22121004。

摘　　要：The Haber-Bosch process for industrial NH_(3) production is energy-intensive with heavy CO_(2) emissions.Electrochemical N_(2) reduction reaction(NRR)is an attractive carbon-neutral alternative for NH_(3) synthesis,while the challenge associated with N_(2) activation highlights the demand for efficient electrocatalysts.Herein,we demonstrate that PdCu nanoparticles with different Pd/Cu ratios anchored on boron nanosheet(PdCu/B)behave as efficient NRR electrocatalysts toward NH_(3) synthesis.Theoretical and experimental results confirm that the highly efficient NH_(3) synthesis can be achieved by regulating the charge transfer between interfaces and forming a symmetry-breaking site,which not only alleviates the hydrogen evolution but also changes the adsorption configuration of N_(2) and thus optimizes the reaction pathway of NRR over the separated Pd sites.Compared with monometallic Pd/B and Cu/B,the PdCu/B with the optimized Pd/Cu ratio of 1 exhibits superior activity and selectivity for NH_(3) synthesis.This study provides new insight into developing efficient catalysts for small energy molecule catalytic conversion via regulating the charge transfer between interfaces and constructing symmetry-breaking sites.

关 键 词：catalyst design electrochemical N_(2)reduction interfacial charge transfer reaction mechanism symmetry-breaking sites 

分 类 号：O64[理学—物理化学]