Reaction environment self-modification on low-coordination Ni 2+ octahedra atomic interface for superior electrocatalyti
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Reaction environment self-modification on low-coordination Ni2+ octahedra atomic interface for superior electrocatalytic overall water splitting Kaian Sun1,2, Lei Zhao1, Lingyou Zeng1, Shoujie Liu2, Houyu Zhu3, Yanpeng Li1, Zheng Chen2, Zewen Zhuang2, Zhaoling Li4, Zhi Liu1, Dongwei Cao3, Jinchong Zhao1, Yunqi Liu1 (), Yuan Pan1 (), and Chen Chen2 () 1
State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China 2 Department of Chemistry, Tsinghua University, Beijing 100084, China 3 College of Science, China University of Petroleum (East China), Qingdao 266580, China 4 State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Textiles, Donghua University, Shanghai 201620, China © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 2 March 2020 / Revised: 1 June 2020 / Accepted: 6 July 2020
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.
KEYWORDS atomic interface effect, overall water splitting, high current density, reaction environment self-modification, density functional theory
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Introduction
Developing sustainable and environment-friendly energy technologies are of critical significance to meet the ever-increasing global energy demands. Electrochemical water splitting, which involves two key processes of cathodic hydrogen evolution reaction (HER) and anodic oxygen evolution reaction (OER), represents a promising alternative to convert electricity produced from intermittent natural resources into chemical energy. To make the water splitting process industrially more feasible, it is of great importance to design bifunctional transition metal electrocatalysts with low cost and high activity for both HER and OER [1].
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