Single Nickel Atom-Modified Phosphorene Nanosheets for Electrocatalytic CO<sub>2</sub> Reduction
Mingyuan Wang, Hui Shi, Ming Tian, Ruowang Chen, Junpeng Shu, Quan Zhang, Yonghu Wang, Cuiyu Li, Neng Wan, Shuangying Lei
Abstract
Nowadays, carbon dioxide (CO2) produced by global energy consumption far exceeds what the environment can absorb. So, the world is seeking a way to control and reduce CO2 emissions. The electrocatalytic CO2 reduction reaction (CRR) can effectively convert this greenhouse gas into energy sources, thus providing a method to solve CO2 emission and energy crisis issues. However, only quite limited catalysts are capable of converting CO2 into high-value C1 products. Herein, four structures of single Ni atom-modified phosphorene, as an electrocatalyst for the CRR, have been studied by first-principles calculations based on density functional theory (DFT). The results show that a single Ni atom adsorbed on monoatomic defective phosphorene (Ni-D-BP) has higher long-term activity and stability, and better CRR selectivity against the hydrogen evolution reaction (HER). In particular, Ni-D-BP shows good selectivity for HCOOH with a limiting potential of −0.31 V. The production of CH3OH and CH4 has the same limiting potential of −0.98 V, indicating that Ni-D-BP also has good catalytic properties for CH3OH or CH4 production. This study can reveal the mechanism of the CRR for single Ni atom-modified phosphorene-based catalysts and provide a way to design electrocatalysts for the CRR on the atomic scale.