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High selectivity of photocatalytic reduction of CO₂ to CO based on terpyridine ligand supported Cu^I metal organic framework.

ABSTRACT: In this work, a 4'-(4-cynaophenyl)-4,2':6',4-terpyridine supported Cu^I MOFs photocatalyst (Cu ^I MOF) was applied to the photocatalytic CO₂ reduction for the first time. The micro-structural and physicochemical properties of the Cu ^I MOF were systematically studied by the powder X-ray diffraction (PXRD), Single crystal X-ray diffraction (SCXRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR), UV-Vis diffuse spectroscopy (UV-vis DRS), ns-level photoluminescence spectra (ns-level PL), Ultraviolet photoelectron spectroscopy (UPS), and N₂ adsorption-desorption test (BET-BJH). Moreover, the in situ diffuse reflectance infrared fourier transform spectroscopy (in situ DRIFTS) was applied to investigate the adsorption and reaction intermediates of photocatalytic CO₂ reduction. As a result, Cu ^I MOF exhibited good performance and outstanding selectivity toward photocatalytic reduction of CO₂ to CO under full-spectrum and visible light illumination. Notably, 100% selective photocatalytic conversion of CO₂ to CO was achieved. Thus, the study presents the high selectivity and CO₂ reduction efficiency of Cu ^I MOF as a potential family of photocatalysts.

SUBMITTER: Zhang WD

PROVIDER: S-EPMC9388720 | biostudies-literature | 2022

REPOSITORIES: biostudies-literature

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High selectivity of photocatalytic reduction of CO2 to CO based on terpyridine ligand supported CuI metal organic framework.

Zhang Wen-Dong WD Wang Yun Y Liang Yi Y Jiang Ai-Lin AL Gong Hao H Tian Xiao-Ying XY Fu Wen-Sheng WS Liao Jia-Zhen JZ Chen Peng P Ma Ying-Zhao YZ

Frontiers in chemistry 20220805

In this work, a 4'-(4-cynaophenyl)-4,2':6',4-terpyridine supported CuI MOFs photocatalyst (Cu I MOF) was applied to the photocatalytic CO2 reduction for the first time. The micro-structural and physicochemical properties of the Cu I MOF were systematically studied by the powder X-ray diffraction (PXRD), Single crystal X-ray diffraction (SCXRD), scanning electron microscope (SEM), X-ray photoelectron spectroscop ...[more]

PMID: 35991597

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Project description:To address the challenge of selectivity toward single products in Cu-catalyzed electrochemical CO2 reduction, one strategy is to incorporate a second metal with the goal of tuning catalytic activity via synergy effects. In particular, catalysts based on Cu modified with post-transition metals (Sn or In) are known to reduce CO2 selectively to either CO or HCOO- depending on their composition. However, it remains unclear exactly which factors induce this switch in reaction pathways and whether these two related bimetal combinations follow similar general structure-activity trends. To investigate these questions systematically, Cu-In and Cu-Sn bimetallic catalysts were synthesized across a range of composition ratios and studied in detail. Compositional and morphological control was achieved via a simple electrochemical synthesis approach. A combination of operando and quasi-in situ spectroscopic techniques, including X-ray photoelectron, X-ray absorption, and Raman spectroscopy, was used to observe the dynamic behaviors of the catalysts' surface structure, composition, speciation, and local environment during CO2 electrolysis. The two systems exhibited similar selectivity dependency on their surface composition. Cu-rich catalysts produce mainly CO, while Cu-poor catalysts were found to mainly produce HCOO-. Despite these similarities, the speciation of Sn and In at the surface differed from each other and was found to be strongly dependent on the applied potential and the catalyst composition. For Cu-rich compositions optimized for CO production (Cu85In15 and Cu85Sn15), indium was present predominantly in the reduced metallic form (In0), whereas tin mainly existed as an oxidized species (Sn2/4+). Meanwhile, for the HCOO--selective compositions (Cu25In75 and Cu40Sn60), the indium exclusively exhibited In0 regardless of the applied potential, while the tin was reduced to metallic (Sn0) only at the most negative applied potential, which corresponds to the best HCOO- selectivity. Furthermore, while Cu40Sn60 enhances HCOO- selectivity by inhibiting H2 evolution, Cu25In75 improves the HCOO- selectivity at the expense of CO production. Due to these differences, we contend that identical mechanisms cannot be used to explain the behavior of these two bimetallic systems (Cu-In and Cu-Sn). Operando surface-enhanced Raman spectroscopy measurements provide direct evidence of the local alkalization and its impact on the dynamic transformation of oxidized Cu surface species (Cu2O/CuO) into a mixture of Cu(OH)2 and basic Cu carbonates [Cux(OH)y(CO3)y] rather than metallic Cu under CO2 electrolysis. This study provides unique insights into the origin of the switch in selectivity between CO and HCOO- pathways at Cu bimetallic catalysts and the nature of surface-active sites and key intermediates for both pathways.

Dataset Information

High selectivity of photocatalytic reduction of CO₂ to CO based on terpyridine ligand supported Cu^I metal organic framework.

Publications

High selectivity of photocatalytic reduction of CO<sub>2</sub> to CO based on terpyridine ligand supported Cu<sup>I</sup> metal organic framework.

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