Single-Atom Pt Anchored on Oxygen Vacancy of Monolayer Ti3C2Tx for Superior Hydrogen Evolution

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2022-01-18 DOI:10.1021/acs.nanolett.1c04809

Jiangjiang Zhang, Erqing Wang, Shiqiang Cui, Shubin Yang, Xiaolong Zou, Yongji Gong*

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引用次数: 49

Abstract

Two-dimensional (2D) MXene-loaded single-atom (SA) catalysts have drawn increasing attention. SAs immobilized on oxygen vacancies (O_V) of MXene are predicted to have excellent catalytic performance; however, they have not yet been realized experimentally. Here Pt SAs immobilized on the O_V of monolayer Ti₃C₂T_x flakes are constructed by a rapid thermal shock technique under a H₂ atmosphere. The resultant Ti₃C₂T_x-Pt_SA 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 mg_Pt^–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 O_V of Ti₃C₂T_x 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.

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单原子Pt锚定在单层Ti3C2Tx的氧空位上，具有优异的析氢性能

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。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

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.