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

Shiqi Peng ¹Yongfang Rao ²Tan Li ³Yufei Zhang ⁴Jun-ji Cao ⁵Shuncheng Lee ⁶Yu Huang⁷

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作者信息

1. 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
2. Department of Environmental Science and Engineering,Xi'an Jiaotong University,Xi'an 710049,China
3. 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
4. School of Environmental and Municipal Engineering,Xi'an University of Architecture and Technology,Xi'an 710055,China
5. School of Human Settlements and Civil Engineering,Xi'an Jiaotong University,Xi'an 710049,China;Institute of Atmospheric Physics,Chinese Academy of Sciences,Beijing 100190,China
6. h Department of Civil and Environmental Engineering,The Hong Kong Polytechnic University,Hong Kong,China
7. 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;CAS Center for Excellence in Quaternary Science and Global Change,Xi'an 710061,China
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Abstract

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.

Key words

ZrO2 nanoparticles/Ir single atoms/Electronic structure/Formaldehyde/Catalytic oxidation

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基金项目

Strategic Priority Research Program of the Chinese Academy of Sciences,China(XDA23010300)

Strategic Priority Research Program of the Chinese Academy of Sciences,China(XDA23010000)

National Science Foundation of China,China(52200137)

National Science Foundation of China,China(21725102)

Plan for"National Youth Talents"and GuangDong Basic and Applied Basic Research Foundation(2021A1515110427)

出版年

2024

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

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