Published: Jan. 1, 2025
Language: Английский
Published: Jan. 1, 2025
Language: Английский
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
6Advanced 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
2Environmental 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
2Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: 508, P. 160993 - 160993
Published: Feb. 28, 2025
Language: Английский
Citations
1Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162084 - 162084
Published: March 1, 2025
Language: Английский
Citations
1Journal 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
1Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 365, P. 124933 - 124933
Published: Dec. 11, 2024
Language: Английский
Citations
6Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124835 - 124835
Published: Nov. 1, 2024
Language: Английский
Citations
5Advanced 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
5Carbon, Journal Year: 2024, Volume and Issue: unknown, P. 119735 - 119735
Published: Oct. 1, 2024
Language: Английский
Citations
3