Selective Photocatalytic Aerobic Oxidation of Methane to Methyl Hydroperoxide by ZnO-Loaded Single-Atomic Ruthenium Oxide Catalyst DOI

Hantao Gong,

Li Zhang, Changzhou Deng

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Photooxidation of CH4 to value-added chemicals with high selectivity offers a promising pathway drive the rational utilization natural gas resources renewable energy under mild conditions. However, owing poor chemoselectivity reactive oxygen radical formation and consecutive side reactions primary products, synthesis peroxide directly from oxidation remains challenging. Here, we report single-atom ruthenium oxide-doped ZnO as highly selective photocatalyst for aerobic CH3OOH. Under optimal conditions, CH3OOH rate over Ru1Ox/ZnO reaches 321 μmol gcat–1 h–1 90.9% simulated solar irradiation. Mechanistic studies reveal that generation •OOH radicals via reduction ability prevent secondary are main advantages Ru1Ox/ZnO, accounting remarkable CH4. The Ru oxide/ZnO catalyst also exhibits alkyl hydroperoxide in photocatalytic low paraffins, which provides solution prepare single-step hydrocarbon substrates.

Language: Английский

Catalyzing Artificial Photosynthesis with TiO2 Heterostructures and Hybrids: Emerging Trends in a Classical yet Contemporary Photocatalyst DOI Open Access
Xiaowen Ruan, Shijie Li,

Chengxiang Huang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: Oct. 11, 2023

Titanium dioxide (TiO

Citations

75

Amide Covalent Bonding Engineering in Heterojunction for Efficient Solar-Driven CO2 Reduction DOI
Weidong Hou, Huazhang Guo, Minghong Wu

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(20), P. 20560 - 20569

Published: Oct. 4, 2023

Inefficient charge separation and slow interfacial reaction dynamics significantly hamper the efficiency of photocatalytic CO2 reduction. Herein, a facile EDC/NHS-assisted linking strategy was developed to enhance in heterojunction photocatalysts. Using this approach, we successfully synthesized amide-bonded carbon quantum dot-g-C3N4 (CQD-CN) The formation amide covalent bonds between CN CQDs CN-CQD facilitates efficient carrier migration, adsorption, activation. Exploiting these advantages, photocatalysts exhibit high selectivity with CO CH4 evolution rates 79.2 2.7 μmol g-1 h-1, respectively. These are about 1.7 3.6 times higher than those CN@CQD bulk CN, Importantly, demonstrate exceptional stability, even after 12 h continuous testing. presence COOH* signal is identified as crucial intermediate species conversion CO. This study presents bonding engineering for developing high-performance solar-driven reduction CO2.

Language: Английский

Citations

70

Selective Photocatalytic Oxidation of Methane to Methanol by Constructing a Rapid O2 Conversion Pathway over Au–Pd/ZnO DOI
Qiang Zhou,

Xiaojie Tan,

Xinyu Wang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(2), P. 955 - 964

Published: Jan. 5, 2024

Photocatalytic oxidation of methane to methanol is an attractive process under mild conditions, nevertheless confronting significant challenges in achieving high conversion and selectivity simultaneously. Herein, we propose a strategy for the direct rapid generation hydroxyl radicals (•OH) from O2 (O2 → *OOH •OH) by rational design Au–Pd/ZnO photocatalyst, skipping water-soluble H2O2 avoiding diffusion. For photocatalytic at ambient temperature, yield CH3OH over optimized 1.0% AuPd0.5/ZnO catalyst were as 81.0 μmol·h–1 88.2%, respectively, exceeding that most reported systems. The formation Au–Pd alloys could improve adsorption cleavage O–O bond *OOH, facilitating efficient •OH increasing selectivity. This work provides some guidance delicate composite photocatalysts selective utilization.

Language: Английский

Citations

34

Engineering triple O-Ti-O vacancy associates for efficient water-activation catalysis DOI Creative Commons
Feng Bi, Qingjie Meng, Yili Zhang

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 20, 2025

Defect engineering can create various vacancy configurations in catalysts by finely tuning the local electronic and geometric structures of active sites. However, achieving precise control identification these defects remains a significant challenge, origin catalysts, especially clustered or associated ones, largely unknown. Herein, we successfully achieve controllable fabrication quantitative triple O-Ti-O associate (VOVTiVO) nanosized Ni-doped TiO2. Experimental theoretical analyses demonstrate that terminal hydroxyls adsorbed at unsaturated cationic sites play an essential role boosting VOVTiVO formation, which enhances H2O dissociation facilitates dissociative OH* deprotonation for defect site regeneration. In contrast, single VO be easily saturated bridging hydroxyl accumulation, leading to gradual decrease number The TiO2 is evidenced its comparable catalytic performance hydrogen evolution reaction hydrodechlorination reactions. Our work highlights importance vacancy-associated presents notable approach designing highly selective efficient H2O-involved enhance manipulating configurations, but controlling them challenging. authors report vacancies TiO2, boost reactions through water

Language: Английский

Citations

5

Radiation-synthesis of covalent bonding heterojunctions for selective solar-driven CO2 reduction DOI
Weidong Hou,

Huazhang Guo,

Kang Wang

et al.

Materials Today, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 1, 2025

Language: Английский

Citations

2

Atomically Dispersed Nickel Anchored on a Nitrogen‐Doped Carbon/TiO2Composite for Efficient and Selective Photocatalytic CH4Oxidation to Oxygenates DOI Creative Commons
Hui Song, Hengming Huang, Xianguang Meng

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(4)

Published: Nov. 30, 2022

Direct photocatalytic oxidation of methane to liquid oxygenated products is a sustainable strategy for valorization at room temperature. However, in this reaction, noble metals are generally needed function as cocatalysts obtaining adequate activity and selectivity. Here, we report atomically dispersed nickel anchored on nitrogen-doped carbon/TiO2 composite (Ni-NC/TiO2 ) highly active selective catalyst photooxidation CH4 C1 oxygenates with O2 the only oxidant. Ni-NC/TiO2 exhibits yield 198 μmol 4 h selectivity 93 %, exceeding that most reported high-performance photocatalysts. Experimental theoretical investigations suggest single-atom Ni-NC sites not enhance transfer photogenerated electrons from TiO2 isolated Ni atoms but also dominantly facilitate activation form key intermediate ⋅OOH radicals, which synergistically lead substantial enhancement both

Language: Английский

Citations

40

Synergy of Ag and AgBr in a Pressurized Flow Reactor for Selective Photocatalytic Oxidative Coupling of Methane DOI Creative Commons
Chao Wang, Xiyi Li, Yifei Ren

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(6), P. 3768 - 3774

Published: March 2, 2023

Oxidation of methane into valuable chemicals, such as C2+ molecules, has been long sought after but the dilemma between high yield and selectivity desired products remains. Herein, is upgraded through photocatalytic oxidative coupling (OCM) over a ternary Ag–AgBr/TiO2 catalyst in pressurized flow reactor. The ethane 35.4 μmol/h with 79% obtained under 6 bar pressure. These are much better than most previous benchmark performance OCM processes. results attributed to synergy Ag AgBr, where serves an electron acceptor promotes charge transfer AgBr forms heterostructure TiO2 not only facilitate separation also avoid overoxidation process. This work thus demonstrates efficient strategy for conversion by both rational design reactor engineering conversion.

Language: Английский

Citations

34

Sustainable Energy Resources for Driving Methane Conversion DOI
Rong Chen, Guo‐Ming Weng

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(36)

Published: Aug. 13, 2023

Abstract The conversion of methane to value‐added chemicals by traditional reforming processes suffers from intensive energy consumption due its particularly strong C─H bonds. Thus, it is urgent optimize the driving force structure for accelerating integration sustainable energy. In this review, advances in energy‐driven are systematically summarized provide a scientific understanding operation/storage concepts, reactor design, technological maturity, system optimization, and remaining issues. Furthermore, essence, economic evaluations, balance, social impacts driven carefully discussed, paving path future course research development. Diversifying mix can play an important role industries, being used as crucial step transition energy, especially combination solar/nuclear with fossil fuels produce chemicals. Additionally, review intends bridge studies development, ultimate goal offering robust framework understand current status guidance design solutions greener future.

Language: Английский

Citations

32

Recent advances on aerobic photocatalytic methane conversion under mild conditions DOI
Yuheng Jiang, Siyang Li, Xiaoyu Fan

et al.

Nano Research, Journal Year: 2023, Volume and Issue: 16(11), P. 12558 - 12571

Published: Oct. 31, 2023

Language: Английский

Citations

30

Selective photocatalytic oxidation of methane to methanol by enhancing H2O2 utilization over Au-Pd/In2O3 DOI
Qiang Zhou, Xinyu Wang,

Tao Xing

et al.

Journal of Catalysis, Journal Year: 2024, Volume and Issue: 429, P. 115289 - 115289

Published: Jan. 1, 2024

Language: Английский

Citations

16