{"title":"非晶化工程与阴离子浸出相结合促进尿素氧化预催化剂重构。","authors":"Ping Li,Han Yang,Zhihong Jiang,Shien Zhao,Wei Qiao,Yuqi Huang,Yu Yu,Jingyun Fang","doi":"10.1002/smll.202507056","DOIUrl":null,"url":null,"abstract":"Ni-based materials have emerged as a class of promising precatalysts for the urea oxidation reaction (UOR), yet inherent structure-related reconstruction behavior of the precatalyst and correlation with electrocatalytic activity are not well-understood, severely hindering rational design of advanced catalysts. Herein, a new type of precatalyst, amorphous Mn-incorporated NiWO4 (a-MnNi-WO4), is constructed via rapid co-precipitation followed by mild heat treatment, and proposed for expediting the UOR. Intriguingly, loose and flexible amorphous phase engineering and leachable WO4 2- incorporation can collaboratively prompt a-MnNi-WO4 to access fast and complete self-reconstruction during UOR, thus generating porous, oxygen-vacancy-enriched, and low-crystalline Mn-doped NiOOH with optimized electronic structure for prompting urea adsorption and the rate-determining step of *COO desorption. Impressively, the a-MnNi-WO4 can deliver admirable UOR behavior and considerably outperform the crystalline counterpart as well as the amorphous ones without WO4 2- or Mn species incorporation, favorably presenting the state-of-the-art level. This work elucidates an in-depth understanding of the reconstruction ability of the precatalyst for promoting the UOR, and material design principle for achieving fast and deep self-reconstruction via amorphization engineering and sacrificial anion etching is expected to extend to construct other advanced electrocatalytic systems.","PeriodicalId":228,"journal":{"name":"Small","volume":"80 1","pages":"e07056"},"PeriodicalIF":12.1000,"publicationDate":"2025-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Amorphization Engineering Coupled with Anion Leaching Boosts Precatalyst Reconstruction for Enhanced Urea Oxidation.\",\"authors\":\"Ping Li,Han Yang,Zhihong Jiang,Shien Zhao,Wei Qiao,Yuqi Huang,Yu Yu,Jingyun Fang\",\"doi\":\"10.1002/smll.202507056\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Ni-based materials have emerged as a class of promising precatalysts for the urea oxidation reaction (UOR), yet inherent structure-related reconstruction behavior of the precatalyst and correlation with electrocatalytic activity are not well-understood, severely hindering rational design of advanced catalysts. Herein, a new type of precatalyst, amorphous Mn-incorporated NiWO4 (a-MnNi-WO4), is constructed via rapid co-precipitation followed by mild heat treatment, and proposed for expediting the UOR. Intriguingly, loose and flexible amorphous phase engineering and leachable WO4 2- incorporation can collaboratively prompt a-MnNi-WO4 to access fast and complete self-reconstruction during UOR, thus generating porous, oxygen-vacancy-enriched, and low-crystalline Mn-doped NiOOH with optimized electronic structure for prompting urea adsorption and the rate-determining step of *COO desorption. Impressively, the a-MnNi-WO4 can deliver admirable UOR behavior and considerably outperform the crystalline counterpart as well as the amorphous ones without WO4 2- or Mn species incorporation, favorably presenting the state-of-the-art level. This work elucidates an in-depth understanding of the reconstruction ability of the precatalyst for promoting the UOR, and material design principle for achieving fast and deep self-reconstruction via amorphization engineering and sacrificial anion etching is expected to extend to construct other advanced electrocatalytic systems.\",\"PeriodicalId\":228,\"journal\":{\"name\":\"Small\",\"volume\":\"80 1\",\"pages\":\"e07056\"},\"PeriodicalIF\":12.1000,\"publicationDate\":\"2025-08-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Small\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/smll.202507056\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Small","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/smll.202507056","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Amorphization Engineering Coupled with Anion Leaching Boosts Precatalyst Reconstruction for Enhanced Urea Oxidation.
Ni-based materials have emerged as a class of promising precatalysts for the urea oxidation reaction (UOR), yet inherent structure-related reconstruction behavior of the precatalyst and correlation with electrocatalytic activity are not well-understood, severely hindering rational design of advanced catalysts. Herein, a new type of precatalyst, amorphous Mn-incorporated NiWO4 (a-MnNi-WO4), is constructed via rapid co-precipitation followed by mild heat treatment, and proposed for expediting the UOR. Intriguingly, loose and flexible amorphous phase engineering and leachable WO4 2- incorporation can collaboratively prompt a-MnNi-WO4 to access fast and complete self-reconstruction during UOR, thus generating porous, oxygen-vacancy-enriched, and low-crystalline Mn-doped NiOOH with optimized electronic structure for prompting urea adsorption and the rate-determining step of *COO desorption. Impressively, the a-MnNi-WO4 can deliver admirable UOR behavior and considerably outperform the crystalline counterpart as well as the amorphous ones without WO4 2- or Mn species incorporation, favorably presenting the state-of-the-art level. This work elucidates an in-depth understanding of the reconstruction ability of the precatalyst for promoting the UOR, and material design principle for achieving fast and deep self-reconstruction via amorphization engineering and sacrificial anion etching is expected to extend to construct other advanced electrocatalytic systems.
期刊介绍:
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology.
Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.