Ling Wang, Kun Zhao, Zhihao Qi, Yonggang Yang, Wei Luo, Wenshu Yang, Longhua Li, Jinhui Hao* and Weidong Shi*,
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The representative low crystalline Ni<sub>2</sub>P (LC-Ni<sub>2</sub>P) possesses a relatively weak surface structure compared with highly crystalline or amorphous Ni<sub>2</sub>P (HC-Ni<sub>2</sub>P or A-Ni<sub>2</sub>P), which contributes abundant oxygen vacancies after the discharge process. The fast discharge behavior of LC-Ni<sub>2</sub>P leads to the uniform distribution of these vacancies and thus endows the inner interface with reactant activating functionality. A high increase in current density of 36.7% is achieved at 2.32 V (vs RHE) for the LC-Ni<sub>2</sub>P electrode. The understanding of the discharge behavior in this study, on different crystalline matrices, presents insights into the establishment of controllable surface reconstruction for an effective oxygen evolution reaction.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":"62 5","pages":"2470–2479"},"PeriodicalIF":4.7000,"publicationDate":"2023-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Crystalline-Dependent Discharge Process of Locally Enhanced Electrooxidation Activity on Ni2P\",\"authors\":\"Ling Wang, Kun Zhao, Zhihao Qi, Yonggang Yang, Wei Luo, Wenshu Yang, Longhua Li, Jinhui Hao* and Weidong Shi*, \",\"doi\":\"10.1021/acs.inorgchem.2c04462\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The state-of-the-art transition-based electrocatalysts in alkaline media generally suffer from unavoidable surface reconstruction during oxygen evolution reaction measurements, leading to the collapse and loss of the crystalline matrix. Low potential discharge offers a gentle way for surface reconstruction and thus realizes the manipulation of the real active site. Nevertheless, the absence of a fundamental understanding focus on this discharge region renders the functional phase, either the crystalline or amorphous matrix, for the controllable reconstruction still undecidable. Herein, we report a scenario to employ different crystalline matrices as electrocatalysts for discharge region reconstruction. The representative low crystalline Ni<sub>2</sub>P (LC-Ni<sub>2</sub>P) possesses a relatively weak surface structure compared with highly crystalline or amorphous Ni<sub>2</sub>P (HC-Ni<sub>2</sub>P or A-Ni<sub>2</sub>P), which contributes abundant oxygen vacancies after the discharge process. The fast discharge behavior of LC-Ni<sub>2</sub>P leads to the uniform distribution of these vacancies and thus endows the inner interface with reactant activating functionality. A high increase in current density of 36.7% is achieved at 2.32 V (vs RHE) for the LC-Ni<sub>2</sub>P electrode. The understanding of the discharge behavior in this study, on different crystalline matrices, presents insights into the establishment of controllable surface reconstruction for an effective oxygen evolution reaction.</p>\",\"PeriodicalId\":40,\"journal\":{\"name\":\"Inorganic Chemistry\",\"volume\":\"62 5\",\"pages\":\"2470–2479\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2023-01-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganic Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.inorgchem.2c04462\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.inorgchem.2c04462","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0
摘要
在析氧反应中,碱性介质中最先进的过渡基电催化剂通常会发生不可避免的表面重构,导致晶体基质的破裂和损失。低电位放电为表面重建提供了一种温和的方法,从而实现了对真实活性部位的操纵。然而,由于缺乏对放电区域的基本理解,使得用于可控重建的功能相(晶体或非晶基体)仍然无法确定。在此,我们报告了一种使用不同晶体基质作为电催化剂来重建放电区域的方案。具有代表性的低晶Ni2P (LC-Ni2P)与高晶Ni2P或非晶Ni2P (HC-Ni2P或a -Ni2P)相比,具有相对较弱的表面结构,在放电过程中具有丰富的氧空位。LC-Ni2P的快速放电行为导致这些空位分布均匀,从而使内部界面具有反应物活化功能。在2.32 V (vs RHE)下,LC-Ni2P电极的电流密度增加了36.7%。本研究中对不同晶体基质的放电行为的理解,为建立有效的析氧反应的可控表面重建提供了见解。
Crystalline-Dependent Discharge Process of Locally Enhanced Electrooxidation Activity on Ni2P
The state-of-the-art transition-based electrocatalysts in alkaline media generally suffer from unavoidable surface reconstruction during oxygen evolution reaction measurements, leading to the collapse and loss of the crystalline matrix. Low potential discharge offers a gentle way for surface reconstruction and thus realizes the manipulation of the real active site. Nevertheless, the absence of a fundamental understanding focus on this discharge region renders the functional phase, either the crystalline or amorphous matrix, for the controllable reconstruction still undecidable. Herein, we report a scenario to employ different crystalline matrices as electrocatalysts for discharge region reconstruction. The representative low crystalline Ni2P (LC-Ni2P) possesses a relatively weak surface structure compared with highly crystalline or amorphous Ni2P (HC-Ni2P or A-Ni2P), which contributes abundant oxygen vacancies after the discharge process. The fast discharge behavior of LC-Ni2P leads to the uniform distribution of these vacancies and thus endows the inner interface with reactant activating functionality. A high increase in current density of 36.7% is achieved at 2.32 V (vs RHE) for the LC-Ni2P electrode. The understanding of the discharge behavior in this study, on different crystalline matrices, presents insights into the establishment of controllable surface reconstruction for an effective oxygen evolution reaction.
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.