{"title":"单原子Pt锚定在单层Ti3C2Tx的氧空位上，具有优异的析氢性能","authors":"Jiangjiang Zhang, Erqing Wang, Shiqiang Cui, Shubin Yang, Xiaolong Zou, Yongji Gong*","doi":"10.1021/acs.nanolett.1c04809","DOIUrl":null,"url":null,"abstract":"<p >Two-dimensional (2D) MXene-loaded single-atom (SA) catalysts have drawn increasing attention. SAs immobilized on oxygen vacancies (O<sub>V</sub>) of MXene are predicted to have excellent catalytic performance; however, they have not yet been realized experimentally. Here Pt SAs immobilized on the O<sub>V</sub> of monolayer Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> flakes are constructed by a rapid thermal shock technique under a H<sub>2</sub> atmosphere. The resultant Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>-Pt<sub>SA</sub> catalyst exhibits excellent hydrogen evolution reaction (HER) performance, including a small overpotential of 38 mV at 10 mA cm<sup>–2</sup>, a high mass activity of 23.21 A mg<sub>Pt</sub><sup>–1</sup>, and a large turnover frequency of 23.45 s<sup>–1</sup> at an overpotential of 100 mV. Furthermore, density functional theory calculations demonstrate that anchoring the Pt SA on the O<sub>V</sub> of Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> helps to decrease the binding energy and the hybridization strength between H atoms and the supports, contributing to rapid hydrogen adsorption–desorption kinetics and high activity for the HER.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6000,"publicationDate":"2022-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"49","resultStr":"{\"title\":\"Single-Atom Pt Anchored on Oxygen Vacancy of Monolayer Ti3C2Tx for Superior Hydrogen Evolution\",\"authors\":\"Jiangjiang Zhang, Erqing Wang, Shiqiang Cui, Shubin Yang, Xiaolong Zou, Yongji Gong*\",\"doi\":\"10.1021/acs.nanolett.1c04809\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Two-dimensional (2D) MXene-loaded single-atom (SA) catalysts have drawn increasing attention. SAs immobilized on oxygen vacancies (O<sub>V</sub>) of MXene are predicted to have excellent catalytic performance; however, they have not yet been realized experimentally. Here Pt SAs immobilized on the O<sub>V</sub> of monolayer Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> flakes are constructed by a rapid thermal shock technique under a H<sub>2</sub> atmosphere. The resultant Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>-Pt<sub>SA</sub> catalyst exhibits excellent hydrogen evolution reaction (HER) performance, including a small overpotential of 38 mV at 10 mA cm<sup>–2</sup>, a high mass activity of 23.21 A mg<sub>Pt</sub><sup>–1</sup>, and a large turnover frequency of 23.45 s<sup>–1</sup> at an overpotential of 100 mV. Furthermore, density functional theory calculations demonstrate that anchoring the Pt SA on the O<sub>V</sub> of Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> helps to decrease the binding energy and the hybridization strength between H atoms and the supports, contributing to rapid hydrogen adsorption–desorption kinetics and high activity for the HER.</p>\",\"PeriodicalId\":53,\"journal\":{\"name\":\"Nano Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.6000,\"publicationDate\":\"2022-01-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"49\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nano Letters\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.nanolett.1c04809\",\"RegionNum\":1,\"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":"Nano Letters","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.nanolett.1c04809","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 49
摘要
二维(2D) mxene负载单原子(SA)催化剂越来越受到人们的关注。预测了在MXene氧空位(OV)上固定化sa具有优异的催化性能;然而，它们尚未在实验中实现。在H2气氛下，采用快速热冲击技术在单层Ti3C2Tx片的OV上构建了固定化Pt SAs。所制得的Ti3C2Tx-PtSA催化剂具有优异的析氢反应性能，在10 mA cm-2下具有38 mV的小过电位，23.21 a mgPt-1的高质量活性，在100 mV过电位下具有23.45 s-1的高周转频率。此外，密度泛函数理论计算表明，将Pt SA锚定在Ti3C2Tx的OV上有助于降低结合能和H原子与载体之间的杂化强度，有助于快速的氢吸附-解吸动力学和较高的HER活性。
Single-Atom Pt Anchored on Oxygen Vacancy of Monolayer Ti3C2Tx for Superior Hydrogen Evolution
Two-dimensional (2D) MXene-loaded single-atom (SA) catalysts have drawn increasing attention. SAs immobilized on oxygen vacancies (OV) of MXene are predicted to have excellent catalytic performance; however, they have not yet been realized experimentally. Here Pt SAs immobilized on the OV of monolayer Ti3C2Tx flakes are constructed by a rapid thermal shock technique under a H2 atmosphere. The resultant Ti3C2Tx-PtSA catalyst exhibits excellent hydrogen evolution reaction (HER) performance, including a small overpotential of 38 mV at 10 mA cm–2, a high mass activity of 23.21 A mgPt–1, and a large turnover frequency of 23.45 s–1 at an overpotential of 100 mV. Furthermore, density functional theory calculations demonstrate that anchoring the Pt SA on the OV of Ti3C2Tx helps to decrease the binding energy and the hybridization strength between H atoms and the supports, contributing to rapid hydrogen adsorption–desorption kinetics and high activity for the HER.
期刊介绍：
Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including:
- Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale
- Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies
- Modeling and simulation of synthetic, assembly, and interaction processes
- Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance
- Applications of nanoscale materials in living and environmental systems
Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.
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