Please use this identifier to cite or link to this item:
https://hdl.handle.net/2440/138794
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Type: | Journal article |
Title: | Acidic CO2-to-HCOOH electrolysis with industrial-level current on phase engineered tin sulfide. |
Author: | Shen, H. Jin, H. Li, H. Wang, H. Duan, J. Jiao, Y. Qiao, S.-Z. |
Citation: | Nature Communications, 2023; 14(1) |
Publisher: | Nature Research (part of Springer Nature) |
Issue Date: | 2023 |
ISSN: | 2041-1723 2041-1723 |
Statement of Responsibility: | Haifeng Shen, Huanyu Jin, HaoboLi, HeruiWang, Jingjing Duan, Yan Jiao, Shi-Zhang Qiao |
Abstract: | Acidic CO2-to-HCOOH electrolysis represents a sustainable route for value-added CO2 transformations. However, competing hydrogen evolution reaction (HER) in acid remains a great challenge for selective CO2-to-HCOOH production, especially in industrial-level current densities. Main group metal sulfides derived S-doped metals have demonstrated enhanced CO2-to-HCOOH selectivity in alkaline and neutral media by suppressing HER and tuning CO2 reduction intermediates. Yet stabilizing these derived sulfur dopants on metal surfaces at large reductive potentials for industrial-level HCOOH production is still challenging in acidic medium. Herein, we report a phase-engineered tin sulfide pre-catalyst (π-SnS) with uniform rhombic dodecahedron structure that can derive metallic Sn catalyst with stabilized sulfur dopants for selective acidic CO2-to-HCOOH electrolysis at industrial-level current densities. In situ characterizations and theoretical calculations reveal the π-SnS has stronger intrinsic Sn-S binding strength than the conventional phase, facilitating the stabilization of residual sulfur species in the Sn subsurface. These dopants effectively modulate the CO2RR intermediates coverage in acidic medium by enhancing *OCHO intermediate adsorption and weakening *H binding. As a result, the derived catalyst (Sn(S)-H) demonstrates significantly high Faradaic efficiency (92.15 %) and carbon efficiency (36.43 %) to HCOOH at industrial current densities (up to -1 A cm-2) in acidic medium. |
Rights: | © The Author(s) 2023 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/. |
DOI: | 10.1038/s41467-023-38497-3 |
Grant ID: | http://purl.org/au-research/grants/arc/FL170100154 http://purl.org/au-research/grants/arc/DP220102596 |
Published version: | http://dx.doi.org/10.1038/s41467-023-38497-3 |
Appears in Collections: | Chemical Engineering publications |
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hdl_138794.pdf | Published version | 2.42 MB | Adobe PDF | View/Open |
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