Recent advances, application and prospect in g-C3N4-based S-scheme heterojunction photocatalysts

Separation and Purification Technology, Journal Year: 2023, Volume and Issue: 330, P. 125302 - 125302

Published: Oct. 12, 2023

Language: Английский

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Dual Atom Catalysts for Energy and Environmental Applications

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(40)

Published: June 7, 2023

The pursuit of high metal utilization in heterogeneous catalysis has triggered the burgeoning interest various atomically dispersed catalysts. Our aim this review is to assess key recent findings synthesis, characterization, structure-property relationship and computational studies dual-atom catalysts (DACs), which cover full spectrum applications thermocatalysis, electrocatalysis photocatalysis. In particular, combination qualitative quantitative characterization with cooperation DFT insights, synergies superiorities DACs compare counterparts, high-throughput catalyst exploration screening machine-learning algorithms are highlighted. Undoubtably, it would be wise expect more fascinating developments field as tunable

Language: Английский

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Atomically Dispersed Silver‐Cobalt Dual‐Metal Sites Synergistically Promoting Photocatalytic Hydrogen Evolution

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

Published: April 25, 2023

Abstract Regulating the coordination environment of single‐atom sites is high necessity to promote catalytic performances photocatalysts. Herein, preparation atomically dispersed Co‐Ag dual‐metal anchored on P‐doped carbon nitride (Co 1 Ag ‐PCN) via supramolecular and solvothermal approaches reported, which demonstrates desirable performance for photocatalytic H 2 evolution from water splitting. The optimal Co ‐PCN catalyst achieves a remarkable hydrogen production rate 1190 µmol g −1 h with an apparent quantum yield (AQY) 1.49% at 365 nm, superior most newly reported metal‐N‐coordinated Systematic experimental characterizations density functional theoretic studies attribute enhanced activity synergistic effect dual exclusive configuration Co‐N 6 Ag‐N C , enhances charge promotes oriented electrons transport metal centers reduced free energy barriers by facilitating formation H* intermediates as key step in evolution. This study reveals versatile strategy tailor electronic structures synergies engineering neighboring environment.

Language: Английский

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Dinuclear metal synergistic catalysis for energy conversion

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(9), P. 3170 - 3214

Published: Jan. 1, 2023

An exclusive review focusing on catalysts exhibiting the dinuclear metal synergistic catalysis (DMSC) effect for energy conversion reactions is presented.

Language: Английский

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Reversed Electron Transfer in Dual Single Atom Catalyst for Boosted Photoreduction of CO₂

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(44)

Published: Aug. 22, 2023

Abstract Photogenerated charge localization on material surfaces significantly affects photocatalytic performance, especially for multi‐electron CO 2 reduction. Dual single atom (DSA) catalysts with flexibly designed reactive sites have received significant research attention photoreduction. However, the transfer mechanism in DSA remains poorly understood. Here, first time, a reversed electron Au and Co is reported. In situ characterizations confirm that CdS nanoparticles (NPs) loaded or atoms, photogenerated electrons are localized around of Au. catalysts, however, delocalized from accumulate atoms. Importantly, combined advanced spectroscopic findings theoretical computation evidence this Au/Co boosts redistribution activation molecules, leading to highly increased reduction, example, exhibits, respectively, ≈2800% 700% greater yields CH 4 compared alone. Reversed can be used practical design boost photoreduction . Findings will benefit researchers manufacturers DSA‐loaded generation solar fuels.

Language: Английский

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Regulating the Local Electronic Structure of Copper Single Atoms with Unsaturated B,O-Coordination for Selective ¹O₂ Generation

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(18), P. 12414 - 12424

Published: Sept. 7, 2023

Generating singlet oxygen (1O2) on single atom catalysts (SACs) in peroxymonosulfate (PMS)-based Fenton-like reactions exhibits great potential for selective degradation of contaminants complex wastewater. Clarifying the structure–activity relationship between electronic structure SACs and 1O2 generation selectivity is crucial precise design efficient catalysts, but it challenging. Herein, Cu with different structures (namely, Cu–O2X, where X = N, S, B, P, O) investigated by density functional theory calculations using adsorption terminal atoms PMS as an activity descriptor. Significantly, affected center which electron-depleted Cu-O2B site a higher atoms. Experimentally, moiety superior catalytic activation, showing nearly 100% ciprofloxacin rate 0.2250 min–1, outperforming those other counterparts. The high attributed to asymmetric accelerating faster electron transfer O–O bond stretching, lowering energy barrier key intermediates toward generation. This work provides broader perspective regulating sites at atomic level catalysts.

Language: Английский

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Highly Efficient Electroreduction of CO₂ to Ethanol via Asymmetric C–C Coupling by a Metal–Organic Framework with Heterodimetal Dual Sites

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(49), P. 26783 - 26790

Published: Nov. 28, 2023

The electroreduction of CO2 into value-added liquid fuels holds great promise for addressing global environmental and energy challenges. However, achieving highly selective yielding multi-carbon oxygenates through the electrochemical reduction reaction (eCO2RR) is a formidable task, primarily due to sluggish asymmetric C-C coupling reaction. In this study, novel metal-organic framework (CuSn-HAB) with unprecedented heterometallic Sn···Cu dual sites (namely, pair SnN2O2 CuN4 bridged by μ-N atoms) was designed overcome limitation. CuSn-HAB demonstrated an impressive Faradic efficiency (FE) 56(2)% eCO2RR alcohols, current density 68 mA cm-2 at low potential -0.57 V (vs RHE). Notably, no significant degradation observed over continuous 35 h operation specified density. Mechanistic investigations revealed that, in comparison copper site, site exhibits higher affinity oxygen atoms. This enhanced plays pivotal role facilitating generation key intermediate *OCH2. Consequently, compared homometallic Cu···Cu (generally ethylene product), were proved be more thermodynamically favorable between *CO *OCH2, leading formation *CO-*OCH2, which ethanol product.

Language: Английский

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Interlayer Spacing Regulation by Single‐Atom Indium^δ+–N₄ on Carbon Nitride for Boosting CO₂/CO Photo‐Conversion

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(35)

Published: May 17, 2023

Abstract Simultaneous optimization on bulk photogenerated‐carrier separation and surface atomic arrangement of catalyst is crucial for reactivity CO 2 photo‐reduction. Rare studies capture the detail that, better than in‐plane regulation, interlayer‐spacing regulation may significantly influence carrier transport bulk‐catalyst thereby affecting its photo‐reduction in g ‐C 3 N 4 . Herein, through a single atom‐assisted thermal‐polymerization process, single‐atom In‐bonded N‐atom (In δ + –N ) (002) crystal planes originally constructed. This In reduces interplanar spacing by electrostatic adsorption, which enhances carriers greatly promotes photoreduction. The photo‐conversion performance this resulted modified superior to other atom loaded carbon nitride catalysts. Moreover, adsorption , *COOH formation energy, optimizes reaction path. It achieves remarkable 398.87 µmol −1 h yield rate, 0.21% apparent quantum efficiency, nearly 100% selectivity without any cocatalyst or sacrificial agent. Through d modulation atom, study provides ground‐breaking insight enhancement from double‐gain view structural control ‐reduction photocatalysts.

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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Cu-Based Materials for Enhanced C2+ Product Selectivity in Photo-/Electro-Catalytic CO2 Reduction: Challenges and Prospects

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

Published: Jan. 4, 2024

Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues the energy shortages. Among materials utilized for catalytic reduction of CO

Language: Английский

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