Selective oxygen vacancy engineering for shrinking the potential barrier of S-scheme heterojunction toward highly efficient photocatalytic CO2 conversion DOI
Yue Huang, Jinfeng Zhang,

Ruzimuradov Olim

et al.

Published: Jan. 1, 2025

Language: Английский

Precision Molecular Engineering of Carbon Nitride for Efficient and Selective Photoreduction of CO2 to C2H6 in Pure Water DOI Open Access

Zihe Chen,

Guixiang Ding,

Zhaoqiang Wang

et al.

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

Published: Feb. 7, 2025

Abstract Photocatalytic CO 2 reduction into high‐value C 2+ products such as H 6 is of great importance but challenging due to their multi‐electron steps and high energy barrier C─C coupling. Moreover, improving its solar‐to‐chemical (STC) conversion efficiency in pure water beyond the current 1% empirical value also a significant challenge. Herein, graphite carbon nitride (g‐C 3 N 4 ) nanosheets with controllable (C) doping nitrogen (N) vacancies (PCCN‐x) are designed through biochar‐tailored protocol for efficiently selectively photo‐converting . The optimal PCCN‐10 photocatalyst enables achievement an exceptional activity 99.14 µmol g −1 h selectivity 80.33% over 20 water. A record STC ≈1.13% solar fuel production from O vapor achieved without any other inputs. Outdoor tests demonstrated impressive ‐to‐C photo‐conversion rate 43.17 water, stable 50 period. Critically, experimental theoretical calculations further confirm pivotal role bridged sites activating molecules promoting formation coupling intermediate ( * OCCO), which very beneficial performance this work photocatalytic fuels paves way large‐scale broader sustainable applications.

Language: Английский

Citations

6
O‐Bridged Co‐Cu Dual‐Atom Catalyst Synergistically Triggers Interfacial Proton‐Coupled Electron Transfer: A New Approach to Sustainable Decontamination DOI Open Access
Qin Dai, Xin Li, Jieyuan Li

et al.

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

Published: Jan. 28, 2025

Abstract Heteroatom‐bridged dual‐atom catalysts (DACs), featuring more flexible active sites and intermetallic interaction, provide an opportunity for sustainable environmental remediation. Herein, innovative oxygen‐bridged Co‐Cu DAC supported on nano‐alumina (CoOCu‐DAC) is fabricated using a straightforward two‐step process. The as‐prepared catalyst significantly enhances both decontamination kinetics peroxymonosulfate (PMS) utilization efficiency by 1–3 orders of magnitude toward monoethanolamine (MEA, p K = 9.5) compared to Co single‐atom (Co‐SAC) bulk metal catalysts, largely outperforms previously reported systems. In‐situ ATR‐FTIR theoretical investigations reveal that the secondary introduction Cu plays multiple important roles: it activates lattice oxygen trigger key proton transfer (PT) MEAH + via nucleophilic attack at interface subsequently favors deprotonated MEA as efficient electron donor accelerate (ET) enhancing orbital overlaps co‐activation O 2 PMS. Such stepwise proton‐coupled (PCET)‐enhanced catalytic pathway mediated CoOCu‐DAC fundamentally different from common route identified in Co‐SAC‐involved Fenton‐like system. established binary QSAR further substantiates universality PCET‐enhanced strategy versatile nitrogen‐containing organic compounds. This study offers new perspective water other related areas catalysis based rationalized design multifunctional atomic level.

Language: Английский

Citations

2
Enhanced CO2 conversion to CO using an S‑scheme 2D/2D WO3/InVO4 photocatalysts DOI
Yanan Chen, Wanchun Xiang, Zizhong Zhang

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: 508, P. 160993 - 160993

Published: Feb. 28, 2025

Language: Английский

Citations

2
From Single-Atom to Dual-Atom: A Universal Principle for the Rational Design of Heterogeneous Fenton-like Catalysts DOI

Shengbo Wang,

Xiuli Hou,

Yichan Li

et al.

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: April 22, 2025

Developing efficient heterogeneous Fenton-like catalysts is the key point to accelerating removal of organic micropollutants in advanced oxidation process. However, a general principle guiding reasonable design highly has not been constructed up now. In this work, total 16 single-atom and 272 dual-atom transition metal/nitrogen/carbon (TM/N/C) for H2O2 dissociation were explored systematically based on high-throughput density functional theory machine learning. It was found that TM/N/C exhibited distinct volcano-type relationship between catalytic activity •OH adsorption energy. The favorable energies range -3.11 ∼ -2.20 eV. Three different descriptors, namely, energetic, electronic, structural found, which can correlate intrinsic properties their activity. Using energy, stability, activation energy as evaluation criteria, two CoCu/N/C CoRu/N/C screened out from candidates, higher than best catalyst due synergistic effect. This work could present conceptually novel understanding inspire structure-oriented viewpoint volcano relationship.

Language: Английский

Citations

2
Polarized microenvironment-modulated covalent organic frameworks with nickel single atoms for enhanced CO2 photoreduction DOI

Piyan Wang,

Ying Dai, Zhenyu Song

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162084 - 162084

Published: March 1, 2025

Language: Английский

Citations

1
Selectivity studies and modification strategies for high-efficiency photocatalytic CO2 reduction to methanol products DOI
Ping Zhang,

Reyila Tuerhong,

Yongchong Yu

et al.

Journal of Materials Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Research on photocatalytic reduction of carbon dioxide (CO 2 ) has extensively progressed.

Language: Английский

Citations

1
Selective Photoconversion of CO2 to C2H4 on Asymmetrical CeO2─Cu2O Interfaces Driven by Oxygen Vacancies DOI Open Access

Lin Chen,

Xiran Yang,

Zhiying He

et al.

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

Published: March 25, 2025

Abstract Photocatalytic conversion of CO 2 into valuable C H 4 is desirable for achieving a carbon‐neutral future, yet faces sluggish kinetics C─C dimerization and insufficient electron deliverability. Herein, an effective top‐down etching route presented to construct interfacial asymmetric oxygen vacancies (Ov) in CeO ─Cu O supported on the copper foam (CeO O/CF). In situ characterizations theoretical calculations demonstrate that nanointerface‐based heterojunctions serve as rapid electron‐transfer pathways, promoting efficiency without need sacrificial agents. Moreover, sites (Ce‐Ov‐Cu) with different charge distributions can effectuate coupling reaction through stabilization key * COCO intermediates, thus making reduction become more favorable process. Accordingly, optimized O/CF demonstrates remarkable performance 93% selectivity toward generation impressive production rate 26.1 µmol g −1 h . Such strongly coupled heterogeneous catalysts finely tailored structure interaction, containing polarized metal at interface, will provide some inspiration constructing efficient photocatalysts convert high value‐added multi‐carbon products solar energy.

Language: Английский

Citations

1
Theoretical design of dual-site metallo-covalent organic frameworks for efficient CO2 photoreduction into C2H4 DOI

K.M Chen,

Ya Wang,

Yuqi Dong

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 365, P. 124933 - 124933

Published: Dec. 11, 2024

Language: Английский

Citations

6
Sulfur vacancy-rich ZnS on ordered microporous carbon frameworks for efficient photocatalytic CO2 reduction DOI

Xiaowu Gao,

Linglong Li,

Ziwei Zhao

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124835 - 124835

Published: Nov. 1, 2024

Language: Английский

Citations

5
Spatial Coupling of Photocatalytic CO2 Reduction and Selective Oxidation on Covalent Triazine Framework/ZnIn2S4 Core–Shell Structures DOI
Decheng Li, Xiang Li,

Mang Zheng

et al.

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

Published: Nov. 25, 2024

Abstract Photocatalytic CO 2 reduction coupled with alcohol oxidation to aldehyde presents a promising strategy for the simultaneous production of fuels and valuable chemicals. The efficiency photocatalytic reactions remains low due poor charge separation, difficulty in activation, uncontrolled compatibility between reactions. This work S‐bridged covalent triazine framework (SCTF) core‐ZnIn S 4 shell photocatalysts selective furfural synthesis at distinct active sites. As evidenced by situ X‐ray photoelectron spectroscopy Kelvin probe force microscopy, photogenerated electrons composite transfer from ZnIn SCTF core, improving separation. Experimental theoretical results confirm that presence pyridine N atoms (Lewis basic sites) enhances adsorption, thereby reducing energy barrier *COOH generation promoting *CO production. Meanwhile, furfuryl deprotonation occur on consuming holes, which turn benefits conversion CO. result, optimized SCTF/ZnIn ‐0.2 core/shell photocatalyst exhibited superior yield 263.5 µmol g −1 95% under simulated sunlight irradiation.

Language: Английский

Citations

5