Review on strategies for improving the added value and expanding the scope of CO₂ electroreduction products

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(10), P. 5149 - 5189

Published: Jan. 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.

Language: Английский

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Enhanced Electrochemical CO₂ Reduction to Formate over Phosphate‐Modified In: Water Activation and Active Site Tuning

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 26, 2024

Electrochemical CO

Language: Английский

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pH‐Universal Electrocatalytic CO₂ Reduction with Ampere‐Level Current Density on Doping‐Engineered Bismuth Sulfide

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(32)

Published: May 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.

Language: Английский

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Poly(triazine imide) Crystals for Efficient CO₂ Photoreduction: Surface Pyridine Nitrogen Dominates the Performance

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 1018 - 1026

Published: Jan. 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.

Language: Английский

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Activating inert non-defect sites in Bi catalysts using tensile strain engineering for highly active CO2 electroreduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 24, 2025

Language: Английский

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Cu-Induced Interfacial Water Engineering of SnO₂ for Durable and Highly Selective CO₂ Electroreduction

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(14), P. 10904 - 10912

Published: July 4, 2024

Language: Английский

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Molecular Enhancement of Direct Electrolysis of Dilute CO₂

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(3), P. 911 - 918

Published: Feb. 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.

Language: Английский

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Direct low concentration CO2 electroreduction to multicarbon products via rate-determining step tuning

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 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.

Language: Английский

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pH‐Universal Electrocatalytic CO₂ Reduction with Ampere‐Level Current Density on Doping‐Engineered Bismuth Sulfide

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(32)

Published: May 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.

Language: Английский

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Pulse Manipulation on Cu-Based Catalysts for Electrochemical Reduction of CO₂

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 13697 - 13722

Published: Aug. 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

Language: Английский

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