{"title":"原位形成的Pt-NiOOH纳米点界面协同催化高效氨硼烷水解","authors":"Shuo Zhang, Yao Chen, Zhenbo Xu, Keju Sun, Xin Xiao, Xiaolei Sun, Yuanyuan Li, Jiong Zhao, Ding Chen and Qiang Xu","doi":"10.1039/D4TA08797F","DOIUrl":null,"url":null,"abstract":"<p >Hydrolysis of ammonia borane (AB) comprising multiple intermediate steps is a representative catalytic reaction for hydrogen generation, usually requiring noble metal Pt as a catalyst. Constructing heterostructures is an effective strategy to improve the catalytic activity while reducing Pt usage. Herein, tailored nanodot–nanodot heterostructures of Pt–Ni(OH)<small><sub><em>x</em></sub></small> on reduced graphene oxide (RGO) are realized by the one-step solvothermal method. It is intriguingly found that local NiOOH nanodots, rather than Ni(OH)<small><sub>2</sub></small>, are <em>in situ</em> formed when encountering Pt on RGO, forming the heterointerface. Subsequently, the optimized Pt–Ni(OH)<small><sub><em>x</em></sub></small>/RGO catalyst exhibits the highest turnover frequency (TOF) of 17 740 min<small><sup>−1</sup></small> based on the Pt loading for hydrogen generation from AB hydrolysis at 303 K, which is 28 times as high as that of Pt/RGO. Theoretical calculations reveal that the heterojunction catalyst promotes the chemisorption and dissociation of water molecules, accelerating H<small><sub>2</sub></small> generation from AB hydrolysis. This one-step solvothermal method to produce the Pt–Ni(OH)<small><sub><em>x</em></sub></small>/RGO catalyst provides a general route to high-performance nanodot–nanodot heterostructure catalysts for various hydrogen-generation catalytic domains.</p>","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":" 13","pages":" 9372-9380"},"PeriodicalIF":9.5000,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic catalysis at in situ-formed Pt–NiOOH nanodot interfaces for highly efficient ammonia borane hydrolysis†\",\"authors\":\"Shuo Zhang, Yao Chen, Zhenbo Xu, Keju Sun, Xin Xiao, Xiaolei Sun, Yuanyuan Li, Jiong Zhao, Ding Chen and Qiang Xu\",\"doi\":\"10.1039/D4TA08797F\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Hydrolysis of ammonia borane (AB) comprising multiple intermediate steps is a representative catalytic reaction for hydrogen generation, usually requiring noble metal Pt as a catalyst. Constructing heterostructures is an effective strategy to improve the catalytic activity while reducing Pt usage. Herein, tailored nanodot–nanodot heterostructures of Pt–Ni(OH)<small><sub><em>x</em></sub></small> on reduced graphene oxide (RGO) are realized by the one-step solvothermal method. It is intriguingly found that local NiOOH nanodots, rather than Ni(OH)<small><sub>2</sub></small>, are <em>in situ</em> formed when encountering Pt on RGO, forming the heterointerface. Subsequently, the optimized Pt–Ni(OH)<small><sub><em>x</em></sub></small>/RGO catalyst exhibits the highest turnover frequency (TOF) of 17 740 min<small><sup>−1</sup></small> based on the Pt loading for hydrogen generation from AB hydrolysis at 303 K, which is 28 times as high as that of Pt/RGO. Theoretical calculations reveal that the heterojunction catalyst promotes the chemisorption and dissociation of water molecules, accelerating H<small><sub>2</sub></small> generation from AB hydrolysis. This one-step solvothermal method to produce the Pt–Ni(OH)<small><sub><em>x</em></sub></small>/RGO catalyst provides a general route to high-performance nanodot–nanodot heterostructure catalysts for various hydrogen-generation catalytic domains.</p>\",\"PeriodicalId\":82,\"journal\":{\"name\":\"Journal of Materials Chemistry A\",\"volume\":\" 13\",\"pages\":\" 9372-9380\"},\"PeriodicalIF\":9.5000,\"publicationDate\":\"2025-02-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Materials Chemistry A\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2025/ta/d4ta08797f\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/ta/d4ta08797f","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
由多个中间步骤组成的硼烷氨(AB)水解是一种具有代表性的催化制氢反应,通常需要贵金属铂作为催化剂。构建异质结构是提高催化活性同时减少铂用量的有效策略。本文通过一步溶热法在还原氧化石墨烯(RGO)上实现了量身定制的铂-镍(OH)x 纳米点-纳米点异质结构。有趣的是,在 RGO 上遇到铂时,局部的 NiOOH 纳米点(而不是 Ni(OH)2)会在原位形成,从而形成异质界面。随后,优化后的 Pt-Ni(OH)x/RGO 催化剂在 303 K 条件下进行 AB 水解制氢时,根据铂负载量,显示出最高的周转频率(TOF),达到 17740 min-1,是 Pt/RGO 催化剂的 28 倍。理论计算显示,异质结催化剂促进了水分子的化学吸附和解离,加速了 AB 水解产生 H2。这种一步溶热法制备 Pt-Ni(OH)x/RGO 催化剂为各种氢气生成催化领域的高性能纳米点-纳米点异质结构催化剂提供了一条通用路线。
Synergistic catalysis at in situ-formed Pt–NiOOH nanodot interfaces for highly efficient ammonia borane hydrolysis†
Hydrolysis of ammonia borane (AB) comprising multiple intermediate steps is a representative catalytic reaction for hydrogen generation, usually requiring noble metal Pt as a catalyst. Constructing heterostructures is an effective strategy to improve the catalytic activity while reducing Pt usage. Herein, tailored nanodot–nanodot heterostructures of Pt–Ni(OH)x on reduced graphene oxide (RGO) are realized by the one-step solvothermal method. It is intriguingly found that local NiOOH nanodots, rather than Ni(OH)2, are in situ formed when encountering Pt on RGO, forming the heterointerface. Subsequently, the optimized Pt–Ni(OH)x/RGO catalyst exhibits the highest turnover frequency (TOF) of 17 740 min−1 based on the Pt loading for hydrogen generation from AB hydrolysis at 303 K, which is 28 times as high as that of Pt/RGO. Theoretical calculations reveal that the heterojunction catalyst promotes the chemisorption and dissociation of water molecules, accelerating H2 generation from AB hydrolysis. This one-step solvothermal method to produce the Pt–Ni(OH)x/RGO catalyst provides a general route to high-performance nanodot–nanodot heterostructure catalysts for various hydrogen-generation catalytic domains.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.