journal article·2023-09-27

Microwave Regenerable Nickel, Zinc Co-doped Nitrogen-Coordinated Porous Carbon Catalyst for Nitrogen Fixation

Peiji Deng, Yixian Liu, Yunliang Liu, Yaxi Li, Ruqiang Wu, Lijun Meng, Kang Liang, Yixiang Gan, Fen Qiao, Naiyun Liu, Zhenhui Kang, Haitao Li

ACS Applied Materials & Interfaces· Volume 15· Issue 38
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Abstract

More than 90% of the global NH 3 synthesis is dominated by the Haber–Bosch process, which consumes 2% of the worldwide energy and generates 1.44% of the global carbon emission. The electrochemical N 2 reduction reaction (NRR) is regarded as an attractive alternative route to produce NH 3 under mild reaction conditions, but the electrocatalysts suffer from the difficulty of N≡N cleavage. In this work, we report a leaf-like MOF-derived Ni/Zn bimetallic co-doped nitrogen-coordinated porous carbon (Ni/Zn-NPC) as a cost-effective NH 3 synthesis electrocatalyst. The resultant electrocatalyst achieved a high NH 3 production rate of 22.68 μg h –1 mg cat –1 at −1.0 V vs a reversible hydrogen electrode (RHE) in a 0.1 M Na 2 SO 4 electrolyte. The Ni/Zn-NPC material can be called a microwave regenerable catalyst because microwave treatment has proven to be a crucial part of the multi-field coupling to detoxify and make the catalyst reactive, further improving its stability. Density functional theory (DFT) was chosen to explore the mechanism of Ni/Zn-NPC for NRR, providing a profound prediction of the structure of the active site and related reaction pathways and revealing that trace Ni doping optimizes the local coordination environment and N 2 adsorption of Zn atoms.
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Research context

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Advanced Photocatalysis Techniques · Nanomaterials for catalytic reactions

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Chemistry and Chemical Engineering, Institute for Energy Research of Jiangsu University, Zhenjiang 212013, Jiangsu, China

Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi University, Nanning 530004, China

School of Chemical Engineering, University of New South Wales, Sydney 2052, New South Wales, Australia

School of Civil Engineering, The University of Sydney, Sydney 2006, New South Wales, Australia

State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, Shanghai 200092, China

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, Jiangsu, China

Macao Institute of Materials Science and Engineering (MIMSE), MUST-SUDA Joint Research Center for Advanced Functional Materials, Macau University of Science and Technology, Taipa 999078, Macao, China

Funding

Guangdong Science and Technology Department · Collaborative Innovation Center of Suzhou Nano Science and Technology · Ministry of Science and Technology of the People's Republic of China · National Key Research and Development Program of China · Jiangsu Provincial Department of Education · Jiangsu University · Natural Science Foundation of Jiangsu Province · Key Research and Development Program of Ningxia · National Natural Science Foundation of China · Higher Education Discipline Innovation Project · Suzhou Key Laboratory of Functional Nano and Soft Materials · Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi University

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