Boosting the Ni–Zn interplay via O/N dual coordination for high‐efficiency CO2 electroreduction
Ying Zhang,
Hailei Jiang,
Anuj Kumar,
Hongchuan Zhang,
Zongge Li,
Tongxin Xu,
Yuan Pan,
Yaqun Wang,
Zhiming Liu,
Guoxin Zhang,
Zifeng Yan
Affiliations
Ying Zhang
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering China University of Petroleum (East China) Qingdao Shandong China
Hailei Jiang
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering China University of Petroleum (East China) Qingdao Shandong China
Anuj Kumar
Department of Chemistry, Institute of Humanities and Applied Science GLA University Mathura India
Hongchuan Zhang
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering China University of Petroleum (East China) Qingdao Shandong China
Zongge Li
College of Chemistry and Chemical Engineering Liaocheng University Liaocheng Shandong China
Tongxin Xu
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering China University of Petroleum (East China) Qingdao Shandong China
Yuan Pan
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering China University of Petroleum (East China) Qingdao Shandong China
Yaqun Wang
Al‐Ion Battery Research Center, College of Energy Storage Technology Shandong University of Science and Technology Qingdao Shandong China
Zhiming Liu
Shandong Engineering Laboratory for Preparation and Application of High‐performance Carbon‐Materials, College of Electromechanical Engineering Qingdao University of Science and Technology Qingdao Shandong China
Guoxin Zhang
Al‐Ion Battery Research Center, College of Energy Storage Technology Shandong University of Science and Technology Qingdao Shandong China
Zifeng Yan
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering China University of Petroleum (East China) Qingdao Shandong China
Abstract Design of supportive atomic sites with a controllably adjusted coordinating environment is essential to advancing the reduction of CO2 to value‐added fuels and chemicals and to achieving carbon neutralization. Herein, atomic Ni (Zn) sites that are uniquely coordinated with ternary Zn (Ni)/N/O ligands were successfully decorated on formamide‐derived porous carbon nanomaterials, possibly forming an atomic structure of Ni(N2O1)‐Zn(N2O1), as studied by combining X‐ray photoelectron spectroscopy and X‐ray absorption spectroscopy. With the mediation of additional O coordination, the Ni–Zn dual site induces significantly decreased desorption of molecular CO. The NiZn‐NC decorated with rich Ni(N2O1)‐Zn(N2O1) sites remarkably gained >97% CO Faraday efficiency over a wide potential range of ‒0.8 to ‒1.1 V (relative to reversible hydrogen electrode). Density functional theory computations suggest that the N/O dual coordination effectively modulates the electronic structure of the Ni–Zn duplex and optimizes the adsorption and conversion properties of CO2 and subsequent intermediates. Different from the conventional pathway of using Ni as the active site in the Ni–Zn duplex, it is found that the Ni‐neighboring Zn sites in the Ni(N2O1)‐Zn(N2O1) coordination showed much lower energy barriers of the CO2 protonation step and the subsequent dehydroxylation step.
