Construction of S-scheme heterojunction for enhanced photocatalytic conversation of NO over dual-defect CeO2−x/g-C3N4−x

Journal of Alloys and Compounds, Год журнала: 2022, Номер 933, С. 167819 - 167819

Опубликована: Ноя. 1, 2022

Язык: Английский

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Toward Unifying the Mechanistic Concepts in Electrochemical CO₂ Reduction from an Integrated Material Design and Catalytic Perspective

Advanced Functional Materials, Год журнала: 2022, Номер 32(51)

Опубликована: Окт. 17, 2022

Electrocatalytic CO2 reduction (eCO2RR) is one of the avenues with most potential toward achieving sustainable energy economy and global climate change targets by harvesting renewable into value-added fuels chemicals. From an industrial standpoint, eCO2RR provides specific advantages over thermochemical photochemical pathways in terms much broader product scope, high specificity, easy adaptability to electricity infrastructure. However, unlike water electrolyzers, lack suitable cathode materials for impedes its commercialization due material design challenges. The current state-of-the-art catalysts suffer largely from low reaction rates, insufficient C2+ selectivity, overpotentials, industrial-scale stability. Overcoming scientific applied technical hurdles commercial realization demands a holistic integration catalytic designs, deep mechanistic understanding, efficient process engineering. Special emphasis on understanding performance outcome sought guide future that can play significant role closing anthropogenic carbon loop. This article integrative approach understand principles robust catalyst superimposed underlying projections which strongly depend experimental conditions viz. choice electrolyte, reactor membrane design, pH solvent, partial pressure CO2.

Язык: Английский

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Simultaneous co‐Photocatalytic CO₂Reduction and Ethanol Oxidation towards Synergistic Acetaldehyde Synthesis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 8, 2023

Photocatalytic conversion of CO2 is great interest but it often suffers sluggish oxidation half reaction and undesired by-products. Here, we report for the first simultaneous co-photocatalytic reduction ethanol towards one identical value-added CH3 CHO product on a rubidium potassium co-modified carbon nitride (CN-KRb). The CN-KRb offers record photocatalytic activity 1212.3 μmol h-1 g-1 with high selectivity 93.3 % production, outperforming all state-of-art photocatalysts. It disclosed that introduced Rb boosts *OHCCHO fromation facilitates desorption, while K promotes adsorption activation. Moreover, H+ stemming from confirmed to participate in process, endowing near ideal overall atomic economy. This work provides new strategy effective use photoexcited electron hole selective sustainable paired into product.

Язык: Английский

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Tweaking Photo CO₂ Reduction by Altering Lewis Acidic Sites in Metalated‐Porous Organic Polymer for Adjustable H₂/CO Ratio in Syngas Production

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(50)

Опубликована: Окт. 24, 2023

Herein, we have specifically designed two metalated porous organic polymers (Zn-POP and Co-POP) for syngas (CO+H2 ) production from gaseous CO2 . The variable H2 /CO ratio of with the highest efficiency was produced in water medium (without an hole scavenger photosensitizer) by utilizing basic principle Lewis acid/base chemistry. Also, observed formation entirely different major products during photocatalytic reduction splitting help catalysts, where CO (145.65 μmol g-1 h-1 (434.7 were preferentially obtained over Co-POP & Zn-POP, respectively. higher electron density/better nature investigated further using XPS, XANES, NH3 -TPD studies, which considerably improve activation capacity. Moreover, structure-activity relationship confirmed via situ DRIFTS DFT demonstrated COOH* intermediate along thermodynamic feasibility while occurred Zn-POP.

Язык: Английский

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Dual Lewis Acid‐Base Sites Regulate Silver‐Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(39)

Опубликована: Авг. 11, 2023

Abstract Highly selective photoreduction of CO 2 to valuable hydrocarbons is great importance achieving a carbon‐neutral society. Precisely manipulating the formation Metal 1 ⋅⋅⋅C=O⋅⋅⋅Metal (M ⋅⋅⋅C=O⋅⋅⋅M ) intermediate on photocatalyst interface most critical step for regulating selectivity, while still significant challenge. Herein, inspired by polar electronic structure feature molecule, we propose strategy whereby Lewis acid‐base dual sites confined in bimetallic catalyst surface are conducive forming M precisely, which can promote selectivity hydrocarbon formation. Employing Ag Cu O 3 nanowires with abundant Cu⋅⋅⋅Ag preferred exposed {110} as model catalyst, 100 % toward into CH 4 has been achieved. Subsequent surface‐quenching experiments and density functional theory (DFT) calculations verify that do play vital role considered be prone convert hydrocarbons. This study reports highly photocatalyst, was designed basis newly proposed precise regulation reaction intermediates. Our findings will stimulate further research dual‐site design reduction

Язык: Английский

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