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π-Sticked Metal‒Organic Monolayers for Single-Metal-Site Dependent CO 2 Photoreduction and Hydrogen Evolution Reaction.

التفاصيل البيبلوغرافية
العنوان: π-Sticked Metal‒Organic Monolayers for Single-Metal-Site Dependent CO 2 Photoreduction and Hydrogen Evolution Reaction.
المؤلفون: Liu Z; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Xie Y; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Liu L; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Cai X; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Yin HQ; Institute for New Energy Materials & Low Carbon Technologies, School of Material Science & Engineering, Tianjin University of Technology, Tianjin, 300384, P. R. China., Zuo M; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Liu Y; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Feng S; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Huang W; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China., Wu D; Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis & Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu, 213164, P. R. China.
المصدر: Small (Weinheim an der Bergstrasse, Germany) [Small] 2024 May; Vol. 20 (18), pp. e2309194. Date of Electronic Publication: 2023 Dec 01.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: Wiley-VCH Country of Publication: Germany NLM ID: 101235338 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1613-6829 (Electronic) Linking ISSN: 16136810 NLM ISO Abbreviation: Small Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة: Original Publication: Weinheim, Germany : Wiley-VCH, c2005-
مستخلص: Hierarchical self-assembly of 2D metal‒organic layers (MOLs) for the construction of advanced functional materials have witnessed considerable interest, due to the increasing atomic utilizations and well-defined atom‒property relationship. However, the construction of atomically precise MOLs with mono-/few-layered thickness through hierarchical self-assembly process remains a challenge, mostly because the elaborate long-range order is difficult to control via conventional noncovalent interaction. Herein, a quadruple π-sticked metal‒organic layer (πMOL) is reported with checkerboard-like lattice in ≈1.0 nanometre thickness, on which the catalytic selectivity can be manipulated for highly efficient CO 2 reduction reaction (CO 2 RR) and hydrogen evolution reaction (HER) over a single metal site. In saturated CO 2 aqueous acetonitrile, Fe-πMOL achieves a highly effective CO 2 RR with the yield of ≈3.98 mmol g ‒1  h ‒1 and 91.7% selectivity. In contrast, the isostructural Co-πMOL as well as mixed metallic FeCo-πMOL exhibits a high activity toward HER under similar conditions. DFT calculations reveal that single metal site exhibits the significant difference in CO 2 adsorption energy and activation barrier, which triggers highly selective CO 2 RR for Fe site and HER for Co site, respectively. This work highlights the potential of supramolecular π … π interaction for constructing monolayer MOL materials to uniformly distribute the single metal sites for artificial photosynthesis.
(© 2023 Wiley‐VCH GmbH.)
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معلومات مُعتمدة: 92161121 National Natural Science Foundation of China
فهرسة مساهمة: Keywords: hierarchical self‐assembly; metal–organic layer; photocatalysis; selectivity; single atom site
تواريخ الأحداث: Date Created: 20231201 Latest Revision: 20240502
رمز التحديث: 20240502
DOI: 10.1002/smll.202309194
PMID: 38039490
قاعدة البيانات: MEDLINE
الوصف
تدمد:1613-6829
DOI:10.1002/smll.202309194