Rapid Charge Transfer Endowed by Heteroatom Doped Z‐Scheme Van Der Waals Heterojunction for Boosting Photocatalytic Hydrogen Evolution DOI Open Access
Weinan Xing,

Weifan Shao,

Yingfu Li

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 23, 2025

Abstract Constructing heterojunctions between phase interfaces represents a crucial strategy for achieving excellent photocatalytic performance, but the absence of sufficient interface driving force and limited charge transfer pathway leads to unsatisfactory separation processes. Herein, doping‐engineering is introduced construct In─N bond‐bridged In 2 S 3 nanocluster modified doped carbon nitride (CN) nanosheets Z‐Scheme van der Waals (VDW) (In /CNS) photocatalyst, preparation process just by one‐step pyrolysis using pre‐coordination confinement method. Specifically, atoms doping enhances bond strength forms high‐quality interfacial linkage which serves as atomic‐level “highway” improving electrons migration, decreasing recombination probability. The detailed characterization results, along with theoretical calculations, confirm that both atom incorporation formation VDW synergistically improve internal electric field. This, in turn, accelerates simultaneously light absorption capacity. Consequently, optimal hydrogen evolution performance In₂S₃/CNS2 160.8 times greater than In₂S₃, 8.2 higher CNS. This study emphasizes role atomic‐scale regulation intrinsic fields heterojunctions, contributing ameliorative performance.

Language: Английский

Cd Single Atom as an Electron Mediator in an S‐Scheme Heterojunction for Artificial Photosynthesis of H2O2 DOI Creative Commons
Xiaowen Ruan,

Minghua Xu,

Chunsheng Ding

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 13, 2025

Abstract Developing conductor‐mediated S‐scheme heterojunction photocatalysts imitating natural photosynthetic systems emerges as a promising approach to hydrogen peroxide (H 2 O ) production. However, achieving precise coupling between two semiconductors with charge shuttle and modulating the interfacial interactions still remain significant bottleneck. Herein, we propose catalyst architecture Cd single atom mediated formed by interfacing CdS TiO nanoparticles. This exhibits an H production rate high 60.33 µmol g −1 min under UV–vis light irradiation, which is attributed efficient transport at interface of thanks S‐scheme. In‐situ X‐ray photoelectron spectroscopy (XPS) electron spin resonance (ESR) spin‐trapping tests confirm transfer route. Femtosecond transient absorption (fs‐TA) other ex‐situ characterizations further corroborate across interface. work offers new perspective on constructing atoms heterojunctions enhance photocatalytic performance.

Language: Английский

Citations

3
Functional Groups‐Dependent Tp‐Based COF/MgIn2S4 S‐Scheme Heterojunction for Photocatalytic Hydrogen Evolution DOI Open Access

Yijun Zhou,

Pengyu Dong, Jinhong Liu

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract An effective technique for improving the photocatalytic activity is functional‐group‐oriented approach of covalent organic frameworks (COFs). However, creation functional groups‐dependent COF‐based S‐scheme heterojunction has seldom been reported. In this study, two distinct Tp‐based COFs with different groups using a solvothermal technique, TpPa‐1 −H and TpPa‐2 −Me (methyl), respectively, synthesized. Moreover, COF/MgIn 2 S 4 (MIS) heterojunctions (i.e., TpPa‐1/MIS TpPa‐2/MIS) are created to clarify dynamics photoinduced charges boost H evolution. Notably, evolution optimum TpPa‐1/MIS‐5% (13.16 mmol g −1 h ) 4.3 times greater than that TpPa‐2/MIS‐5% (3.05 ), which attributed in could slow down interfacial photogenerated electron‐transfer make its surface less hydrophilic, resulting lower over TpPa‐2/MIS‐5%. On contrary, remarkable associated fast electron transfer from MIS due hydrophilic TpPa‐1, induced stronger internal electric field motivated by construction heterojunction.

Language: Английский

Citations

3
Topology Control of Covalent Organic Frameworks with Interlaced Unsaturated 2D and Saturated 3D Units for Boosting Electrocatalytic Hydrogen Peroxide Production DOI

Han Wu,

Lili Li,

Hongni Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 13, 2024

Abstract Modulating the electronic state of multicomponent covalent organic framework (COF) electrocatalysts is crucial for enhancing catalytic activity. However, effect dimensionality on their physicochemical functionalities still lacking. Herein, we report an interlaced unsaturated 2D and saturated 3D strategy to develop multicomponent‐regulated COFs with tunable gradient high selectivity activity electrocatalysis. Compared two‐component model COFs, 2D/3D locally irregular dimensions structures are more practical in optimizing intrinsic electrode surface reaction mass transfer. Remarkably, 2D‐inserted TAE‐COF regulates adsorption mode OOH* species supply a favorable dynamic pathway H 2 O process, thereby achieving excellent production rate 8.50 mol g cat −1 h . Moreover, utilizing theoretical calculation situ ATR‐FTIR experiment, found that central carbon atom tetraphenyl‐based unit (site‐1 site‐6) potential active sites. This operating ability reactants dimensionality‐interconnected building blocks provides idea designing durable efficient electrocatalysts.

Language: Английский

Citations

16
Bi4O5Br2/COF S-Scheme Heterojunctions for Boosting H2O2 Photoproduction under Air and Pure Water DOI
Jieyu Yue,

Zi‐Xian Pan,

Peng Yang

et al.

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(9), P. 3932 - 3940

Published: July 26, 2024

Photosynthesizing H2O2 by the oxygen reduction reaction (ORR) and water oxidation (WOR) is a promising green avenue for generation but limited charge carrier recombination rate sluggish kinetics. Herein, Bi4O5Br2/COF step-scheme (S-scheme) heterojunction (named BIT) created first time covalent organic frameworks (TTD-COF) Bi4O5Br2, with an increased separation efficiency photosynthetic activity. Under air pure water, BIT6 exhibits highest production of 5221 μmol g–1 h–1, which 20 1.7 times greater than that individual Bi4O5Br2 TTD-COF. Subsequent mechanism analysis reveals photosynthesizes through overpowering indirect 2e– ORR paths (O2–O2• ––H2O2 O2–O2• ––O21–H2O2) weak direct WOR pathways. Moreover, in situ photogeneration process can be accompanied degradation antibiotics. This study offers in-depth insights into COF-based S-scheme heterojunctions enhanced photoproduction.

Language: Английский

Citations

13
In Situ Construction of Hollow Coral‐Like Porous S‐Doped g‐C3N4/ZnIn2S4 S‐Scheme Heterojunction for Efficient Photocatalytic Hydrogen Evolution DOI Creative Commons
Tianyu Wang,

Xuanlin Pan,

Minyi He

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 3, 2024

The rational design of visible-light-responsive catalysts is crucial for converting solar energy into hydrogen to promote sustainable development. In this work, a C─S─C bond introduced g-C

Language: Английский

Citations

12
Improving Charge Carrier Separation through S-Scheme-Based 2D–2D WS2/Sulfur-Doped g-C3N4 Heterojunctions for a Superior Photocatalytic O2 Reduction Reaction DOI

Kundan Kumar Das,

Upali Aparajita Mohanty, Ritik Mohanty

et al.

ACS Applied Energy Materials, Journal Year: 2024, Volume and Issue: 7(15), P. 6360 - 6375

Published: Aug. 1, 2024

Hydrogen peroxide (H2O2) generation via a photocatalytic O2 reduction reaction has been considered an economically efficient and environmentally friendly synthesis method. However, the productivity of H2O2 production is restricted because sluggish kinetics fast recombination photoinduced excitons. Therefore, superior two-dimensional (2D)–2D WS2/sulfur-doped g-C3N4 (WSCN) hybrid material was successfully fabricated to address associated limitations through combination wet impregnation calcination techniques for production. The effective anchoring WS2 nanoplates onto sulfur-doped (SCN) nanosheets facilitates separation excitons with sturdy redox properties, which attributable establishment S-scheme heterojunctions between SCN W–S bonding as substantiated by X-ray photoelectron spectroscopy (XPS) analysis. bond at interface acts bridge charge segregation pathways. Among all, 2.5 WSCN displays exceptional 817 μmol, 7.9- 2.68-fold higher than those pristine SCN, respectively. solar-to-chemical conversion efficiency found be 0.24%, whereas apparent quantum yield estimated 3.19% 420 nm irradiation. improved activity figured out cathodic photocurrent −1.51 mA cm–2 delayed excitons, supported photoluminescence electrochemical impedance measurements. charge-transfer pathway well validated radical scavenging experiment work function, evaluated from VB-XPS analysis in situ XPS measurement. This research offers paradigmatic idea constructing photocatalyst generation.

Language: Английский

Citations

12
S‐Scheme Heterojunction Fabricated from Covalent Organic Framework and Quantum Dot for Enhanced Photosynthesis of Hydrogen Peroxide from Water and Air DOI
Xiaolin Ma,

Senzhi Li,

Ying Gao

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 16, 2024

Abstract Covalent organic frameworks (COFs) with stable crystalline porous structures and flexible assembly properties contribute to the direct photocatalytic synthesis of H 2 O meet growing global demand. To address challenges insufficient redox capacity photogenerated carrier recombination COFs, S‐scheme heterojunction is constructed from COFs quantum dots (QDs) improve production . Herein, 0D ZnCdS QDs (ZCS) uniformly anchor on surface a 2D conjugated tetrathiafulvalene‐based COF (TT‐COF), affording TT‐COF/ZCS. Formation effectively prevents agglomeration ZCS, modulates energy band structure TT‐COF, enhances migration carriers ability. As total consequence, optimized (TZ‐40) able afford in yield up 5171 µmol g −1 h under visible light irradiation , much higher than those for 2520 2647 The present result demonstrates great potential COFs/QDs‐based heterojunctions applications including production.

Language: Английский

Citations

11
Reticular Materials for Photocatalysis DOI
Kang Sun, Yunyang Qian, Dandan Li

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 27, 2024

Abstract Photocatalysis leverages solar energy to overcome the thermodynamic barrier, enabling efficient chemical reactions under mild conditions. It can greatly reduce reliance on traditional sources and has attracted significant research interest. Reticular materials, including metal‐organic frameworks (MOFs) covalent organic (COFs), represent a class of crystalline materials constructed from molecular building blocks linked by coordination bonds, respectively. function as heterogeneous catalysts, combining well‐defined structures high tailorability akin homogeneous catalysts. In this review, regulation light absorption, charge separation, surface in photocatalytic process through precise molecular‐level design based features reticular is elaborated. Notably, for MOFsmicroenvironment modulation around catalytic sites affects performance delved, with emphasis their unique dynamic flexible microenvironments. For COFs, inherent excitonic effects due fully nature discussed highlight strategies regulate charge‐ and/or energy‐transfer‐mediated photocatalysis. Finally, current challenges future directions field, aiming provide comprehensive understanding how be optimized enhanced photocatalysis discussed.

Language: Английский

Citations

11
Inhibited superoxide‐induced halide oxidation with a bioactive factor for stabilized inorganic perovskite solar cells DOI Creative Commons
Xingxing Duan, Jialong Duan,

Naimin Liu

et al.

SusMat, Journal Year: 2024, Volume and Issue: 4(4)

Published: July 29, 2024

Abstract Active oxygen highly affects the efficiency and stability of perovskite solar cells (PSCs) owing to capacity either passivate defects or decompose lattice. To better understand in‐depth interaction, we demonstrate for first time that photooxidation mechanism in all‐inorganic film dominates phase deterioration kinetics by forming superoxide species presence light oxygen, which is significantly different from organic‒inorganic hybrid even tin‐based perovskites. In perovskites, prefer oxidize longer weaker Pb‒I bond PbO I 2 , leaving much stable CsPbBr 3 phase. From this chemical proof‐of‐concept, employ an organic bioactive factor, Tanshinone IIA, as a sweeper enhance environmental tolerance inorganic perovskite, serving “skincare” agent anti‐aging organisms. Combined with another key point on healing defective lattice, best carbon‐based CsPbI Br cell delivers high 15.12% superior against light, humidity, heat attacks. This method also applicable p‒i‒n inverted (Cs 0.05 MA FA 0.9 )Pb(I 0.93 0.07 ) 23.46%. These findings not only help us decomposition mechanisms depth but provide potential strategy advanced PSC platforms.

Language: Английский

Citations

10
Construction of floating photothermal-assisted S-scheme heterojunction with enhanced photocatalytic degradation of tetracycline: Insights into mechanisms, degradation pathways and toxicity assessment DOI
Yahong Zhou,

Delu Cao,

Rongyu Zhang

et al.

Journal of Environmental Management, Journal Year: 2024, Volume and Issue: 370, P. 122586 - 122586

Published: Sept. 18, 2024

Language: Английский

Citations

10