Encapsulation of Highly Dispersed Au NPs by Strong Metal–Support Interactions in Porous Titania Nanoplates for Efficient Electrosynthesis of H2O2

Author:

He Yilei1,Wei Yanze23,Wang Zumin23,Xia Tian1,Rao Fu1,Song Zhifan1,Yu Ranbo1ORCID

Affiliation:

1. Department of Physical Chemistry School of Metallurgical and Ecological Engineering University of Science & Technology Beijing 30th Xueyuan Road, Haidian Beijing 100083 China

2. State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences 1 North 2nd Street, Zhongguancun, Haidian Beijing 100190 China

3. Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of Sciences 1 North 2nd Street, Zhongguancun, Haidian Beijing 100190 China

Abstract

AbstractTuning the electrocatalytic selectivity and long‐term stability for industrially significant, yet reactively unfavorable products, remains a challenge in oxygen reduction. Herein, the Au/TiO2 catalysts with strong metal–support interactions (SMSI) are designed and synthesized through an in situ auto‐reduction of Au‐modified Ti‐MOF. Highly dispersed ultra‐low loading of Au NPs strongly capsulated in porous TiO2 substrate, together with conductive carbon derivated from MOFs, enables Au/TiO2 electrocatalysts to achieve excellent H2O2 electrosynthesis through the two‐electron oxygen reduction reaction (2e ORR). Au(1.0)/TiO2 (0.52 wt% Au loading) exhibited a high selectivity of 90%, a remarkable Faradaic efficiency of 98%, and 72.2 mg L−1 h−1 H2O2 production. Highly dispersed Au NPs promote active site exposure, while the conductive carbon and the porous superstructure enhance mass diffusion. Notably, the SMSI between Au NPs and TiO2 substrate leads to superb stability (over 168 h) of the electrocatalysts, as it ensures continuous electronic interactions. Experimental characterizations and density functional theory (DFT) simulations further revealed that the SMSI effect medicates the activation of the *OOH intermediate formation and the d‐band center, which are conductive to 2e ORR. Moreover, this strategy provides a potential way toward high‐performance electrocatalysts in flow system devices for continuously purifying sewage and chemical bleaching in extreme environments.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Beijing Municipality

National Key Research and Development Program of China

Publisher

Wiley

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