Piezo‐Electrocatalysis for CO₂ Reduction Driven by Vibration

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(27)

Published: June 2, 2022

Abstract With rising CO 2 emissions caused by the massive consumption of fossil fuels, it is highly desirable to develop strategies that adopt renewable energy convert into value‐added chemical feedstocks. Over past decades, photocatalytic reduction using light has attracted considerable attention. However, advanced photocatalysis techniques cannot exert their action where unavailable. Here, a method for on basis vibration‐driven piezoelectricity yield piezo‐electrocatalysis effect which requires mechanical vibration rather than light, proposed. Under mild and sacrificial agent‐free conditions, piezoelectric BaTiO 3 catalyst provides suitable piezo‐potential overcome redox potential with maximum 63.3 µmol g −1 , achieving reactivity comparable those photocatalysts. The piezo‐electrocatalytic reaction adds new avenue in addition existing expanding scope utilization promote carbon neutrality.

Language: Английский

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Photochromic single atom Ag/TiO₂ catalysts for selective CO₂ reduction to CH₄

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(2), P. 518 - 530

Published: Dec. 7, 2023

A new all-in-one design concept of constructing photochromic single atom photocatalysts is proposed to achieve both high activity and selectivity photocatalytic CO 2 -to-CH 4 conversion.

Language: Английский

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Amide Covalent Bonding Engineering in Heterojunction for Efficient Solar-Driven CO₂ Reduction

ACS Nano, Journal Year: 2023, Volume and Issue: 17(20), P. 20560 - 20569

Published: Oct. 4, 2023

Inefficient charge separation and slow interfacial reaction dynamics significantly hamper the efficiency of photocatalytic CO2 reduction. Herein, a facile EDC/NHS-assisted linking strategy was developed to enhance in heterojunction photocatalysts. Using this approach, we successfully synthesized amide-bonded carbon quantum dot-g-C3N4 (CQD-CN) The formation amide covalent bonds between CN CQDs CN-CQD facilitates efficient carrier migration, adsorption, activation. Exploiting these advantages, photocatalysts exhibit high selectivity with CO CH4 evolution rates 79.2 2.7 μmol g-1 h-1, respectively. These are about 1.7 3.6 times higher than those CN@CQD bulk CN, Importantly, demonstrate exceptional stability, even after 12 h continuous testing. presence COOH* signal is identified as crucial intermediate species conversion CO. This study presents bonding engineering for developing high-performance solar-driven reduction CO2.

Language: Английский

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Decade Milestone Advancement of Defect-Engineered g-C3N4 for Solar Catalytic Applications

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Jan. 4, 2024

Over the past decade, graphitic carbon nitride (g-C

Language: Английский

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Selective CO₂ Photoreduction to Acetate at Asymmetric Ternary Bridging Sites

ACS Nano, Journal Year: 2023, Volume and Issue: 17(5), P. 4922 - 4932

Published: Feb. 17, 2023

Photoreduction of CO2 is a promising strategy to synthesize value-added fuels or chemicals and realize carbon neutralization. Noncopper catalysts are seldom reported generate C2 products, the selectivity over these low. Here, we design rich-interface, heterostructured In2O3/InP (r-In2O3/InP) for highly competitive photocatalytic CO2-to-CH3COOH conversion with productivity 96.7 μmol g–1 > 96% along water oxidation O2 in pure (no sacrificial agent) under visible light irradiation. The hard X-ray absorption near-edge structure (XANES) shows that formation r-In2O3/InP isogenesis cation adjusts coordination environment via interface engineering forms O–In–P polarized sites at interface. In situ FT-IR Raman spectra identify key intermediates OCCO* acetate production high selectivity. Density functional theory (DFT) calculations reveal rich promotes C–C coupling form products because imbalanced adsorption energies two atoms. This work reports an interesting indium-based photocatalyst selective photoreduction strict solution irradiation conditions provides significant insights into fabricating interfacial polarization promote process.

Language: Английский

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Simultaneous CO₂and H₂O Activation via Integrated Cu Single Atom and N Vacancy Dual‐Site for Enhanced CO Photo‐Production

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(28)

Published: April 23, 2023

Abstract Photocatalytic conversion of CO 2 into fuels using pure water as the proton source is immense potential in simultaneously addressing climate‐change crisis and realizing a carbon‐neutral economy. Single‐atom photocatalysts with tunable local atomic configurations unique electronic properties have exhibited outstanding catalytic performance past decade. However, given their single‐site features they are usually only amenable to activations involving single molecules. For photoreduction entailing complex activation dissociation process, designing multiple active sites on photocatalyst for both reduction H O still daunting challenge. Herein, it precisely construct Cu single‐atom centers two‐coordinated N vacancies dual CN (Cu 1 /N 2C V‐CN). Experimental theoretical results show that promote chemisorption via accumulating photogenerated electrons, V enhance O, thereby facilitating from COO* COOH*. Benefiting dual‐functional sites, V‐CN exhibits high selectivity (98.50%) decent production rate 11.12 µmol g −1 h . An ingenious atomic‐level design provides platform integrating modified catalyst deterministic identification property during process.

Language: Английский

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Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: Synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 466, P. 143287 - 143287

Published: May 2, 2023

The creation of an isotype phase junction has been recognized as effective means improving the spatial charge separation and migration in g-C3N4 materials. Nevertheless, due to a lack electrostatic control internal electric field, heterojunction alone is incapable providing sufficient driving force maximize carrier transfer. Herein, we present interface engineering strategy for co-integrating p-n heterojunctions fabricate g-C3N4/g-C3N4 nanohybrids using facile ultrasonic-assisted self-assembly method. coherent boundary between two distinct phases demonstrates that intimate 2D interfacial contact can be easily established by π-π stacking interactions because their high structural similarities low lattice strain. Furthermore, compatible well-matched electronic band structures led staggered type II alignment lateral heterojunction, which confers resulting composite with strong redox ability, efficient exciton dissociation, desirable optoelectronic characteristics beyond those constituents. Essentially, work tandem create robust built-in allowing steering directional electron from BCN CNx. Benefiting these merits, BCN/CNx nanohybrid manifested remarkable CH4 generation photocatalytic CO2 reduction, outperforming its CNx counterparts 1.91 6.88-fold, respectively. midgap states induced nitrogen defects also pose positive effect on improved photoactivity binary acting reservoir mediate transfer further impede recombination. This proof-of-concept study highlights significance flow manipulation utilization enhancement.

Language: Английский

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Constructing atomic surface concaves on Bi5O7Br nanotube for efficient photocatalytic CO2 reduction

Nano Energy, Journal Year: 2023, Volume and Issue: 109, P. 108305 - 108305

Published: Feb. 26, 2023

Language: Английский

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Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: July 11, 2023

Electrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due their versatile industrial applications. However, selectively reducing ethylene is still challenging as the additional energy required for C-C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding key steps preferred pathways/conditions, well rational design novel catalysts production have been regarded approaches achieving highly efficient selective CO2RR. In this review, we first illustrate CO2RR (e.g., adsorption/activation, formation *CO intermediate, step), offering conversion ethylene. Then alternative pathways conditions competitive products (C1 other C2+ products) investigated, guiding further development generation. Engineering strategies Cu-based CO2RR-ethylene summarized, correlations mechanism/pathways, engineering selectivity elaborated. Finally, major challenges perspectives research area proposed future practical

Language: Английский

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Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO2 Reduction

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 16(1)

Published: Nov. 6, 2023

We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO

Language: Английский

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