Exploring P-(Fe,V)-Codoped Metastable-Phase β-NiMoO4 for Improving the Performance of Overall Water Splitting

IF 4.7 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry Pub Date : 2025-01-23 DOI:10.1021/acs.inorgchem.4c0223310.1021/acs.inorgchem.4c02233

Yuxuan Kong, Qingqing Guo, Dengke Xiong, Ning Chai, Qiao Jiang, Tianyu Chen and Fei-Yan Yi*,

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Abstract

It is especially essential to develop high-performance and low-cost nonprecious metal catalysts for large-scale hydrogen production. A large number of electrochemical catalysts composited by transition metal centers has been reported; however, it is still a great challenge to design and manipulate target electrocatalysts to realize high overall water-splitting activity at the atomic level. Herein, we develop totally new P-(Fe,V)-codoped metastable-phase β-NiMoO₄. As an electrocatalyst, it can realize oxygen evolution at only 163 mV and hydrogen evolution at only 44 mV at 10 mA cm^–2. It, as both an anode and a cathode, is fabricated into a cell for overall water splitting, which has an ultralow voltage value of 1.48 V to drive a current density of 10 mA cm^–2 and can remain stable for at least 100 h. In the target electrode, the P element plays three important roles: (1) it can stabilize the metastable-phase structure of β-NiMoO₄; (2) it can further optimize the electronic structure; and (3) it can provide more active sites. The synergistic effect for multimetal centers with different redox couples is key for the great improvement of catalytic activity. The related mechanism is discussed in detail.

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探索P-(Fe，V)-共掺杂亚稳态相β-NiMoO4对提高整体水裂解性能的影响

开发高性能、低成本的非贵金属催化剂对于大规模制氢尤为重要。过渡金属中心复合的电化学催化剂已被大量报道；然而，如何设计和操作目标电催化剂，在原子水平上实现高的整体水分解活性仍然是一个很大的挑战。在此，我们开发了全新的P-（Fe，V）共掺杂亚稳相β-NiMoO4。作为电催化剂，在10 mA cm-2下，析氧速率仅为163 mV，析氢速率仅为44 mV。它作为阳极和阴极，被制作成一个整体水分解的电池，具有1.48 V的超低电压值，驱动10 mA cm-2的电流密度，并可保持至少100 h的稳定。在目标电极中，P元素起着三个重要作用：(1)稳定β-NiMoO4的亚稳相结构；(2)可进一步优化电子结构；(3)能提供更多的活性位点。多金属中心与不同氧化还原对之间的协同作用是提高催化活性的关键。详细讨论了相关机理。

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来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.