Regulating the interfacial charge transfer and constructing symmetry‐breaking sites for the enhanced N2 electroreduction activity
Xiaoxue Zhang,
Yuehan Cao,
Zhen‐Feng Huang,
Shishi Zhang,
Chengguang Liu,
Lun Pan,
Chengxiang Shi,
Xiangwen Zhang,
Ying Zhou,
Guidong Yang,
Ji‐Jun Zou
Affiliations
Xiaoxue Zhang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Yuehan Cao
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
Zhen‐Feng Huang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Shishi Zhang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Chengguang Liu
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Lun Pan
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Chengxiang Shi
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Xiangwen Zhang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Ying Zhou
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
Guidong Yang
XJTU‐Oxford International Joint Laboratory for Catalysis, School of Chemical Engineering and Technology Xi'an Jiaotong University Xi'an Shaanxi China
Ji‐Jun Zou
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University Tianjin China
Abstract The Haber–Bosch process for industrial NH3 production is energy‐intensive with heavy CO2 emissions. Electrochemical N2 reduction reaction (NRR) is an attractive carbon‐neutral alternative for NH3 synthesis, while the challenge associated with N2 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 NH3 synthesis. Theoretical and experimental results confirm that the highly efficient NH3 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 N2 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 NH3 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.
