Regulating the interfacial charge transfer and constructing symmetry‐breaking sites for the enhanced N<sub>2</sub> 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
Abstract
Abstract 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.