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Nano Research

Article Title

Reaction environment self-modification on low-coordination Ni2+ octahedra atomic interface for superior electrocatalytic overall water splitting

Authors

Kaian Sun, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China Department of Chemistry, Tsinghua University, Beijing 100084, China
Lei Zhao, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Lingyou Zeng, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Shoujie Liu, Department of Chemistry, Tsinghua University, Beijing 100084, China
Houyu Zhu, College of Science, China University of Petroleum (East China), Qingdao 266580, China
Yanpeng Li, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Zheng Chen, Department of Chemistry, Tsinghua University, Beijing 100084, China
Zewen Zhuang, Department of Chemistry, Tsinghua University, Beijing 100084, China
Zhaoling Li, State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Textiles, Donghua University, Shanghai 201620, China
Zhi Liu, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Dongwei Cao, College of Science, China University of Petroleum (East China), Qingdao 266580, China
Jinchong Zhao, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Yunqi Liu, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Yuan Pan, State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
Chen Chen, Department of Chemistry, Tsinghua University, Beijing 100084, China

Keywords

atomic interface effect, overall water splitting, high current density, reaction environment self-modification, density functional theory

Abstract

Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion. In this regard, meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecularscale are vitally necessary. Herein, a coordination environment inheriting strategy is presented for designing low-coordination Ni2+ octahedra (L-Ni-8) atomic interface at a high concentration (4.6 at.%). Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode. To improve the efficiency of using the self-modification reaction environment at L-Ni-8, all of the structural features, including high atom economy, mass transfer, and electron transfer, are integrated together from atomic-scale to macro-scale. At high current density of 500 mA/cm2, the samples synthesized at gram-scale can deliver low hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) overpotentials of 262 and 348 mV, respectively.

Graphical Abstract

Publisher

Tsinghua University Press

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