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journal article·2023-03Open access

Ammonia Electrosynthesis with a Stable Metal‐Free 2D Silicon Phosphide Catalyst

Chade Lv, Ning Jia, Yumin Qian, Shanpeng Wang, Xuechun Wang, Wei Yu, Chuntai Liu, Hongge Pan, Qiang Zhu, Jianwei Xu, Xutang Tao, Kian Ping Loh, Can Xue, Qingyu Yan

Small· Volume 19· Issue 10
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Source abstract

Abstract

Abstract Metal‐free 2D phosphorus‐based materials are emerging catalysts for ammonia (NH3) production through a sustainable electrochemical nitrogen reduction reaction route under ambient conditions. However, their efficiency and stability remain challenging due to the surface oxidization. Herein, a stable phosphorus‐based electrocatalyst, silicon phosphide (SiP), is explored. Density functional theory calculations certify that the N2 activation can be realized on the zigzag Si sites with a dimeric end‐on coordinated mode. Such sites also allow the subsequent protonation process via the alternating associative mechanism. As the proof‐of‐concept demonstration, both the crystalline and amorphous SiP nanosheets (denoted as C‐SiP NSs and A‐SiP NSs, respectively) are obtained through ultrasonic exfoliation processes, but only the crystalline one enables effective and stable electrocatalytic nitrogen reduction reaction, in terms of an NH3 yield rate of 16.12 µg h−1 mgcat.−1 and a Faradaic efficiency of 22.48% at −0.3 V versus reversible hydrogen electrode. The resistance to oxidization plays the decisive role in guaranteeing the NH3 electrosynthesis activity for C‐SiP NSs. This surface stability endows C‐SiP NSs with the capability to serve as appealing electrocatalysts for nitrogen reduction reactions and other promising applications.
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Research context

NanomaterialsCatalysis & surfaces

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Advanced Photocatalysis Techniques · MXene and MAX Phase Materials

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

Affiliations

School of Materials Science and Engineering Nanyang Technological University Singapore 639798 Singapore

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 P. R. China

State Key Laboratory of Crystal Materials Shandong University Jinan 250100 P. R. China

Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement Ministry of Education School of Physics Beijing Institute of Technology Beijing 100081 P. R. China

Department of Chemistry National University of Singapore Singapore 117543 Singapore

Key Laboratory of Materials Processing and Mold Ministry of Education Zhengzhou University Zhengzhou 450002 P. R. China

Institute of Science and Technology for New Energy Xi'an Technological University Xi'an 710021 P. R. China

Institute of Materials Research and Engineering A*STAR 2 Fusionopolis Way, Innovis, #08‐03 Singapore 138634 Singapore

Institute of Sustainability for Chemicals, Energy and Environment Agency for Science, Technology and Research (A*STAR) Jurong Island Singapore 627833 Singapore

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