Electronic Structure Regulated Nickel-Cobalt Bimetal Phosphide Nanoneedles for Efficient Overall Water Splitting

Author:

Xu Heyang1,She Xilin1,Li Haolin1,Wang Chuanhui1,Chen Shuai2,Diao Lipeng34,Lu Ping1,Li Longwei1,Tan Liwen1ORCID,Sun Jin1,Zou Yihui1

Affiliation:

1. State Key Laboratory of Bio-Fibers and Eco-Textiles, Shandong Collaborative Innovation Center of Marine Biobased Fibers and Ecological Textiles, Institute of Marine Biobased Materials, School of Environmental Science and Engineering, Qingdao University, Qingdao 266071, China

2. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China

3. Qingdao Hanxing New Materials Co., Ltd., Qingdao 266109, China

4. School of Material Science and Engineering, State Key Laboratory of Bio-Fibers and Eco-Textiles, Qingdao University, Qingdao 266071, China

Abstract

Transition metal phosphides (TMPs) have been widely studied for water decomposition for their monocatalytic property for anodic or cathodic reactions. However, their bifunctional catalytic activity still remains a major challenge. Herein, hexagonal nickel-cobalt bimetallic phosphide nanoneedles with 1–3 μm length and 15–30 nm diameter supported on NF (NixCo2−xP NDs/NF) with adjusted electron structure have been successfully prepared. The overall alkaline water electrolyzer composed of the optimal anode (Ni0.67Co1.33P NDs/NF) and cathode (Ni1.01Co0.99P NDs/NF) provide 100 mA cm−2 at 1.62 V. Gibbs Free Energy for reaction paths proves that the active site in the hydrogen evolution reaction (HER) is Ni and the oxygen evolution reaction (OER) is Co in NixCo2−xP, respectively. In the HER process, Co-doping can result in an apparent accumulation of charge around Ni active sites in favor of promoting HER activity of Ni sites, and ΔGH* of 0.19 eV is achieved. In the OER process, the abundant electron transfer around Co-active sites results in the excellent ability to adsorb and desorb *O and *OOH intermediates and an effectively reduced ∆GRDS of 0.37 eV. This research explains the regulation of electronic structure change on the active sites of bimetallic materials and provides an effective way to design a stable and effective electrocatalytic decomposition of alkaline water.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Shandong Province

Taishan Scholars Program, and the State Key Laboratory of Bio-Fibers and Eco-Textiles

Qingdao University

Publisher

MDPI AG

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