Exceptional Cocatalyst‐Free Photo‐Enhanced Piezocatalytic Hydrogen Evolution of Carbon Nitride Nanosheets from Strong In‐Plane Polarization

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(24)

Published: May 8, 2021

Abstract Utilizing mechanical energy to produce hydrogen is emerging as a promising way generate renewable energy, but challenged by low efficiency and scanty cognition. In this work, graphitic carbon nitride (g‐C 3 N 4 ) with an atomically thin sheet‐like structure applied for prominent piezocatalytic photo‐enhanced H 2 production. It revealed that the anomalous piezoelectricity in g‐C originates from strong in‐plane polarization along ‐axis, contributed superimposed polar tri‐s‐triazine units flexoelectric effect derived structured triangular cavities, which provides powerful electrochemical driving force water reduction reaction. Furthermore, charge transfer enables nanosheets reserve more energized charges fully participate reaction at surface reactive sites enriched strain‐induced vacancies. Without any cocatalysts, exceptional photo‐piezocatalytic evolution rate of 12.16 mmol g −1 h delivered nanosheets, far exceeding previously reported piezocatalysts photocatalysts. Further, high pure‐water‐splitting performance production value‐added oxidation product O via photo‐piezocatalysis also disclosed. This work not only exposes potential piezo‐semiconductor catalytic evolution, breaks new ground conversion solar photomediated

Language: Английский

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Single-atom catalysts for photocatalytic energy conversion

Joule, Journal Year: 2022, Volume and Issue: 6(1), P. 92 - 133

Published: Jan. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Language: Английский

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2D Graphitic Carbon Nitride for Energy Conversion and Storage

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(34)

Published: June 19, 2021

Abstract Graphitic carbon nitride (g‐C 3 N 4 ) have attracted great attention in the field of energy conversion and storage due to its unique layered structure, tunable bandgap, metal‐free characteristic, high physicochemical stability, easy accessibility. 2D g‐C nanosheets features short charge/mass transfer path, abundant reactive sites functionalization, which are beneficial optimizing their performance different fields. However, reviews comprehensive applications for rare. Herein, this review first introduces properties bulk nanosheets, then summarizes synthetic strategies detail, such as thermal oxidation etching, chemical exfoliation, ultrasonication‐assisted liquid phase vapor deposition, others. Emphasis is focused on rational design development diversified storage, including photocatalytic H 2 evolution, CO reduction, electrocatalytic O alkali‐metal ion batteries, lithium‐metal lithium–sulfur metal‐air supercapacitors. Finally, current challenges perspectives discussed.

Language: Английский

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Synergistic Polarization Engineering on Bulk and Surface for Boosting CO₂ Photoreduction

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(33), P. 18303 - 18308

Published: May 31, 2021

Abstract Sluggish charge kinetics and low CO 2 affinity seriously inhibit photoreduction. Herein, the synchronous promotion of separation Bi 4 Ti 3 O 12 is realized by coupling corona poling surface I‐grafting. Corona enhances ferroelectric polarization aligning domains direction, which profoundly promotes transfer along opposite directions across bulk. Surface I‐grafting forms a local electric field for further separating carriers provides abundant active sites to enhance adsorption. The two modifications cooperatively increase , maximize efficiency photogenerated charges, resulting in an enhanced production rate 15.1 μmol g −1 h (nearly 9 times) with no sacrificial agents or cocatalysts. This work discloses that ion grafting can promote photoreduction synergistic way.

Language: Английский

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Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: May 25, 2022

Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion selectivity. Herein, visible irradiation (420 nm), synergy of palladium (Pd) atom cocatalyst oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h-1 C1 oxygenates, with selectivity primary products (CH3OH CH3OOH) up 82.5%. Mechanism investigation elucidates that such induced dedicated function Pd single atoms boosting hole electron transfer, respectively. O2 proven be only source for CH3OH production, while H2O acts as promoter efficient ·OH production facilitates product desorption indicated DFT modeling. This work thus provides new understandings simultaneous regulation activity cocatalysts vacancies.

Language: Английский

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Photocatalytic hydrogen peroxide evolution: What is the most effective strategy?

Nano Energy, Journal Year: 2022, Volume and Issue: 104, P. 107906 - 107906

Published: Oct. 19, 2022

Language: Английский

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All-solid-state direct Z-scheme NiTiO₃/Cd_0.5Zn_0.5S heterostructures for photocatalytic hydrogen evolution with visible light

Journal of Materials Chemistry A, Journal Year: 2021, Volume and Issue: 9(16), P. 10270 - 10276

Published: Jan. 1, 2021

The construction of NiTiO3/Cd0.5Zn0.5S heterostructures is presented as all-solid-state direct Z-scheme photocatalysts for the efficient and stable hydrogen production under visible light. hybrids are assembled by growing Cd0.5Zn0.5S nanoparticles on surface NiTiO3 nanorods via a co-precipitation hydrothermal coupled method. compositional structural features composites fully disclosed diverse physicochemical characterizations. revealed to effectively capture optical spectrum in region well enhance transfer separation photogenerated charge carriers through Z-schematic pathway. Consequently, optimized photocatalyst shows high H2 rate 1058 μmol h−1 (26.45 mmol g−1), which independent any cocatalysts (such Pt), together with apparent quantum yield (AQY) 34% monochromatic light irradiation at 420 nm. Besides, also exhibit stability evolution photocatalysis mainly due fact that migration can enable consumption light-induced holes prevent photocorrosion effect. Finally, possible photocatalytic mechanism over based results band structures, density functional theory (DFT) calculations electron spin resonance (ESR) tests.

Language: Английский

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Understanding the unique S-scheme charge migration in triazine/heptazine crystalline carbon nitride homojunction

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 3, 2023

Understanding charge transfer dynamics and carrier separation pathway is challenging due to the lack of appropriate characterization strategies. In this work, a crystalline triazine/heptazine carbon nitride homojunction selected as model system demonstrate interfacial electron-transfer mechanism. Surface bimetallic cocatalysts are used sensitive probes during in situ photoemission for tracing S-scheme photogenerated electrons from triazine phase heptazine phase. Variation sample surface potential under light on/off confirms dynamic transfer. Further theoretical calculations an interesting reversal path light/dark conditions, which also supports experimental evidence transport. Benefiting unique merit electron transfer, shows significantly enhanced activity CO2 photoreduction. Our work thus provides strategy probe mechanisms design delicate material structures towards efficient

Language: Английский

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Defect engineering in metal sulfides for energy conversion and storage

Coordination Chemistry Reviews, Journal Year: 2021, Volume and Issue: 448, P. 214147 - 214147

Published: Aug. 27, 2021

Language: Английский

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Steering the behavior of photogenerated carriers in semiconductor photocatalysts: a new insight and perspective

Journal of Materials Chemistry A, Journal Year: 2021, Volume and Issue: 9(42), P. 23765 - 23782

Published: Jan. 1, 2021

The current semiconductor photocatalysts only exhibit unsatisfactory photocatalytic efficiency, due to the easy recombination of photogenerated carriers. Regulating separation and transfer carriers reducing are essential for improving catalytic efficiency photocatalysts. is produced by attraction Coulomb force. Consequently, requires an additional driving force counteract However, exploring mechanism carrier regulation from perspective has received sporadic attention. This review firstly starts fundamental impairment performance. Then it focuses on several main strategies regulating behavior aspect carriers, including heterojunction design，construction intramolecular donor-acceptor (D-A) system, exciton regulation, electron spin regulation. Subsequently, advanced characterization techniques latest developments theoretical calculations migration have been introduced. In end, we summarize challenges put forward prospects future development

Language: Английский

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