Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(36)
Опубликована: Июнь 17, 2024
Copper (Cu)-based catalysts have established their unique capability for yielding wide value-added products from CO
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(36)
Опубликована: Июнь 17, 2024
Copper (Cu)-based catalysts have established their unique capability for yielding wide value-added products from CO
Язык: Английский
Chemical Society Reviews, Год журнала: 2024, Номер 53(10), С. 5149 - 5189
Опубликована: Янв. 1, 2024
This review summarizes promising strategies including the design of catalysts and construction coupled electrocatalytic reaction systems, aimed at achieving selective production various products from CO 2 electroreduction.
Язык: Английский
Процитировано
84Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(27)
Опубликована: Апрель 26, 2024
Electrochemical CO
Язык: Английский
Процитировано
23Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)
Опубликована: Май 27, 2024
Abstract The practical application of the electrocatalytic CO 2 reduction reaction (CO RR) to form formic acid fuel is hindered by limited activation molecules and lack universal feasibility across different pH levels. Herein, we report a doping‐engineered bismuth sulfide pre‐catalyst (BiS‐1) that S partially retained after electrochemical reconstruction into metallic Bi for RR formate/formic with ultrahigh performance wide range. best BiS‐1 maintains Faraday efficiency (FE) ~95 % at 2000 mA cm −2 in flow cell under neutral alkaline solutions. Furthermore, catalyst shows unprecedentedly high FE (~95 %) current densities from 100 1300 acidic Notably, density can reach 700 while maintaining above 90 membrane electrode assembly electrolyzer operate stably 150 h 200 . In situ spectra functional theory calculations reveals doping modulates electronic structure effectively promotes formation HCOO* intermediate generation. This work develops efficient stable electrocatalysts sustainable production.
Язык: Английский
Процитировано
22ACS Catalysis, Год журнала: 2025, Номер unknown, С. 1018 - 1026
Опубликована: Янв. 2, 2025
Polymeric carbon nitrides (PCNs), usually the melon phase, have been extensively applied as photocatalysts for CO2 reduction; however, their performance is still unsatisfactory. The condensed allotrope, namely, poly(triazine imide) (PTI) with extended conjugation and a crystallized structure, indeed holds more favorable compositional structural advantages photocatalytic reduction but remains to be fully exploited. Herein, hexagonal prism-shaped PTI crystals were synthesized developed high-performance photocatalyst reduction. With Co(bpy)32+ cocatalyst, exhibit CO evolution rate of 44 μmol h–1 (i.e., 1467 g–1 h–1) 93% selectivity, markedly superior that counterpart. Moreover, manifest an apparent quantum efficiency 12.9% at 365 nm, representing state-of-the-art value by PCN CO2-to-CO without using noble metals. surface pyridine N species are exposed active sites dominate activation conversion, which, together high crystallinity facilitate charge separation transport, endows efficiency. In situ diffuse reflectance infrared Fourier transform spectroscopy determines key intermediates during reaction and, consequently, constructs possible mechanism.
Язык: Английский
Процитировано
8Nature Communications, Год журнала: 2025, Номер 16(1)
Опубликована: Фев. 24, 2025
Язык: Английский
Процитировано
3ACS Catalysis, Год журнала: 2024, Номер 14(14), С. 10904 - 10912
Опубликована: Июль 4, 2024
Язык: Английский
Процитировано
13ACS Energy Letters, Год журнала: 2024, Номер 9(3), С. 911 - 918
Опубликована: Фев. 9, 2024
Producing chemicals and fuels via direct electrolysis of dilute CO2 derived from industrial point sources can improve the economic feasibility technology, yet it suffers many challenges owing to unfavorable mass transport, reaction thermodynamics, kinetics. Here we report a molecular enhancement strategy for stream with 10% concentration in typical flue gas, using commercially available cobalt phthalocyanine (CoPc) catalyst. A poly(4-vinylpyridine) (P4VP)-modified CoPc electrode exhibits remarkable CO partial current density 252 mA cm–2 Faradaic efficiency 90% under feed, 2.24-fold higher than that bare electrode. The integration molecule P4VP modifier abundant pyridine moieties creates microenvironment sequentially capturing activating CO2, thus resulting impressive electrocatalytic performance. presented paves way utilization gas.
Язык: Английский
Процитировано
10Nature Communications, Год журнала: 2024, Номер 15(1)
Опубликована: Ноя. 29, 2024
Direct converting low concentration CO2 in industrial exhaust gases to high-value multi-carbon products via renewable-energy-powered electrochemical catalysis provides a sustainable strategy for utilization with minimized separation and purification capital energy cost. Nonetheless, the electrocatalytic conversion of dilute into value-added chemicals (C2+ products, e.g., ethylene) is frequently impeded by rate weak carbon intermediates' surface adsorption strength. Here, we fabricate range Cu catalysts comprising fine-tuned Cu(111)/Cu2O(111) interface boundary density crystal structures aimed at optimizing rate-determining step decreasing thermodynamic barriers adsorption. Utilizing engineering, attain Faradaic efficiency (51.9 ± 2.8) % partial current (34.5 6.4) mA·cm−2 C2+ feed condition (5% v/v), comparing state-of-art electrolysis. In contrast prevailing belief that activation ( $${{CO}}_{2}+{e}^{-}+\, * \,\to {}^{ }{CO}_{2}^{-}$$ ) governs reaction rate, discover that, under conditions, shifts generation *COOH $${}^{ } {{CO}}_{2}^{-}+{H}_{2}O\to {COOH}+{{OH}}^{-}({aq})$$ Cu0/Cu1+ boundary, resulting better production performance. The development operate resembling waste holds promise reduction. authors report vacuum calcination approach regulating on Cu-based can electro-catalyze low-concentration CO2.
Язык: Английский
Процитировано
9Angewandte Chemie, Год журнала: 2024, Номер 136(32)
Опубликована: Май 27, 2024
Abstract The practical application of the electrocatalytic CO 2 reduction reaction (CO RR) to form formic acid fuel is hindered by limited activation molecules and lack universal feasibility across different pH levels. Herein, we report a doping‐engineered bismuth sulfide pre‐catalyst (BiS‐1) that S partially retained after electrochemical reconstruction into metallic Bi for RR formate/formic with ultrahigh performance wide range. best BiS‐1 maintains Faraday efficiency (FE) ~95 % at 2000 mA cm −2 in flow cell under neutral alkaline solutions. Furthermore, catalyst shows unprecedentedly high FE (~95 %) current densities from 100 1300 acidic Notably, density can reach 700 while maintaining above 90 membrane electrode assembly electrolyzer operate stably 150 h 200 . In situ spectra functional theory calculations reveals doping modulates electronic structure effectively promotes formation HCOO* intermediate generation. This work develops efficient stable electrocatalysts sustainable production.
Язык: Английский
Процитировано
8ACS Catalysis, Год журнала: 2024, Номер unknown, С. 13697 - 13722
Опубликована: Авг. 30, 2024
Electrocatalytic carbon dioxide reduction (CO2RR) over Cu-based catalysts has emerged as a promising strategy for value-added artificial cycling, addressing the current climate and energy challenges. However, product selectivity long-term stability of are limited by their instability at constant potential. Recent advancements in pulsed techniques aim to overcome these limitations, enhancing industrial feasibility CO2RR systems. This review critically examines recent research progress catalysts, offering comprehensive synthesis findings. Key pulse parameters characterization strategies explored uncover mechanisms behind enhanced performance. The focus is on surface reconstruction, encompassing regeneration stabilization Cu oxidation states alongside morphological evolution, while also discussing microenvironment changes, including local CO2 concentration, pH, ionic arrangement. intricate modulation mode, potential, duration performance elucidated, highlighting interconnections. Finally, we identify prevailing challenges propose future directions achieving environmentally friendly economically viable cycling. By providing insightful perspectives optimizing CO2RR, this paves way developing more efficient robust catalytic
Язык: Английский
Процитировано
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