Regulating the electronic structure of Ir single atoms by ZrO2 nanoparticles for enhanced catalytic oxidation of formaldehyde at room temperature

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外文摘要：Developing low-loading single-atom catalysts with superior catalytic activity and selectivity in formalde-hyde(HCHO)oxidation at room temperature remains challenging.Herein,ZrO2 nanoparticles cou-pled low-loading Ir single atoms in N-doped carbon(Ir1-N-C/ZrO2)was prepared.The optimal Ir1-N-C/ZrO2 with 0.25 wt％ Ir loading delivers the high HCHO removal and conversion efficiency(>95％ )at 20℃,which is higher than that over Ir1-N-C with the same Ir loading.The specific rate can reach 1285.6 mmol gIr-1 h-1,surpassing the Ir based catalysts reported to date.Density functional theory cal-culation results and electron spin resonance spectra indicate that the introduction of ZrO2 nanoparticles modulate the electronic structure of the Ir single atoms,promoting O2 activation to·O2-.Moreover,the Ir-C-Zr channel is favorable for the dissociation of·O2-to active oxygen atom(O),and further acceler-ates the transformation of HCHO and intermediates(dioxymethylene and formates)to CO2 and H2O.This work provides a facile strategy to design low-loading single-atom catalysts with high catalytic activity toward HCHO oxidation.

外文关键词：

ZrO2 nanoparticlesIr single atomsElectronic structureFormaldehydeCatalytic oxidation

作者：

Shiqi Peng、Yongfang Rao、Tan Li、Yufei Zhang、Jun-ji Cao、Shuncheng Lee、Yu Huang

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作者单位：

Key Laboratory of Aerosol Chemistry&Physics,State Key Laboratory of Loess and Quaternary Geology(SKLLQG),Institute of Earth Environment,Chinese Academy of Sciences(CAS),Xi'an 710061,China

School of Human Settlements and Civil Engineering,Xi'an Jiaotong University,Xi'an 710049,China

Department of Environmental Science and Engineering,Xi'an Jiaotong University,Xi'an 710049,China

Faculty of Chemical Engineering,Kunming University of Science and Technology,Kunming 650500,China

School of Environment and Energy,South China University of Technology,Guangzhou 51006,China

School of Environmental and Municipal Engineering,Xi'an University of Architecture and Technology,Xi'an 710055,China

Institute of Atmospheric Physics,Chinese Academy of Sciences,Beijing 100190,China

h Department of Civil and Environmental Engineering,The Hong Kong Polytechnic University,Hong Kong,China

CAS Center for Excellence in Quaternary Science and Global Change,Xi'an 710061,China

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基金：

Strategic Priority Research Program of the Chinese Academy of Sciences,ChinaStrategic Priority Research Program of the Chinese Academy of Sciences,ChinaNational Science Foundation of China,ChinaNational Science Foundation of China,ChinaPlan for"National Youth Talents"and GuangDong Basic and Applied Basic Research Foundation

项目编号：

XDA23010300XDA2301000052200137217251022021A1515110427

出版年：

2024

DOI：

10.1016/j.cclet.2023.109219

中国化学快报(英文版)

中国化学会

中国化学快报(英文版)

CSTPCD

影响因子：0.771

ISSN：1001-8417

年,卷(期)：2024.35(7)