PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors DOI Creative Commons
Xiyi Li, Chao Wang, Jianlong Yang

et al.

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

Published: Oct. 10, 2023

Methane activation by photocatalysis is one of the promising sustainable technologies for chemical synthesis. However, current efficiency and stability process are moderate. Herein, a PdCu nanoalloy (~2.3 nm) was decorated on TiO2, which works efficient, stable, selective photocatalytic oxidative coupling methane at room temperature. A high conversion rate 2480 μmol g-1 h-1 to C2 with an apparent quantum ~8.4% has been achieved. More importantly, photocatalyst exhibits turnover frequency number 116 12,642 respect PdCu, representing record among all processes (λ > 300 operated temperature, together long over 112 hours. The as hole acceptor, in Pd softens weakens C-H bond Cu decreases adsorption energy products, leading long-time stability.

Language: Английский

Role of oxygen vacancy in metal oxides for photocatalytic CO2 reduction DOI
Wenbin Jiang,

Hongyi Loh,

Beverly Qian Ling Low

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 321, P. 122079 - 122079

Published: Oct. 17, 2022

Language: Английский

Citations

219
Internal quantum efficiency higher than 100% achieved by combining doping and quantum effects for photocatalytic overall water splitting DOI
Youzi Zhang, Yuke Li,

Xu Xin

et al.

Nature Energy, Journal Year: 2023, Volume and Issue: 8(5), P. 504 - 514

Published: April 10, 2023

Language: Английский

Citations

160
Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts DOI Creative Commons
Xiyi Li, Chao Li, Youxun Xu

et al.

Nature Energy, Journal Year: 2023, Volume and Issue: 8(9), P. 1013 - 1022

Published: Aug. 17, 2023

Abstract Photocatalytic oxidative coupling of methane (OCM) produces C 2 molecules that can be used as building blocks for synthesis fuels and chemicals. However, the yield rate selectivity products are still moderate due to stable nature molecules. Here we develop a Au nanocluster-loaded TiO photocatalyst by sputtering approach, achieving high conversion 1.1 mmol h −1 , ~90% apparent quantum efficiency 10.3 ± 0.6%. The /C 2+ is on same order magnitude benchmark thermal catalysts in OCM processes operated at temperature (>680 °C). nanoparticles shown prolong photoelectron lifetimes factor 66 O reduction, together with acting hole acceptor catalytic centre promote adsorption, C–H activation C–C coupling. This work underscores importance multifunctional co-catalysts mechanistic understanding improve photocatalytic OCM.

Language: Английский

Citations

92
Rapid dissociation of high concentration excitons between [Bi2O2]2+ slabs with multifunctional N-Bi-O sites for selective photoconversion into CO DOI
Guosheng Zhou,

Yangrui Xu,

Liang Chen

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 335, P. 122892 - 122892

Published: May 18, 2023

Language: Английский

Citations

72
Selective Photocatalytic Oxidative Coupling of Methane via Regulating Methyl Intermediates over Metal/ZnO Nanoparticles DOI
Pu Wang, Run Shi, Yunxuan Zhao

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(23)

Published: April 7, 2023

Abstract Methane conversion to higher hydrocarbons requires harsh reaction conditions due high energy barriers associated with C−H bond activation. Herein, we report a systematic investigation of photocatalytic oxidative coupling methane (OCM) over transition‐metal‐loaded ZnO photocatalysts. A 1 wt % Au/ZnO delivered remarkable C 2 ‐C 4 hydrocarbon production rate 683 μmol g −1 h (83 selectivity) under light irradiation excellent photostability two days. The metal type and its interaction strongly influence the selectivity toward C−C products. Photogenerated Zn + ‐O − sites enable CH activation methyl intermediates (*CH 3 ) migrating onto adjacent nanoparticles. nature *CH ‐metal controls OCM In case Au, strong d‐σ orbital hybridization reduces metal‐C−H angles steric hindrance, thereby enabling efficient coupling. Findings indicate center may be suitable descriptor for predicting product during metal/ZnO

Language: Английский

Citations

71
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

71
Chelated Ion‐Exchange Strategy toward BiOCl Mesoporous Single‐Crystalline Nanosheets for Boosting Photocatalytic Selective Aromatic Alcohols Oxidation DOI
Wei Li, Yumeng Mao, Zhilin Liu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(18)

Published: Feb. 21, 2023

The photoresponse and photocatalytic efficiency of bismuth oxychloride (BiOCl) are greatly limited by rapid recombination photogenerated carriers. construction porous single-crystal BiOCl photocatalyst can effectively alleviate this issue provide accessible active sites. Herein, a facile chelated ion-exchange strategy is developed to synthesize mesoporous single-crystalline nanosheets (BiOCl MSCN) using acetic acid ammonia solution respectively as chelating agent ionization promoter. strong chelation between acetate ions Bi3+ introduces into the precipitated product exchange with Cl- ions, resulting in large lattice mismatch, strain release, formation void-like mesopores. prepared MSCN exhibits excellent catalytic performance 99% conversion 98% selectivity for oxidation benzyl alcohol benzaldehyde superior general adaptability various aromatic alcohols. theoretical calculations characterizations confirm that mainly attributed abundant oxygen vacancies, plenty adsorption/active sites fast charge transport path without grain boundaries.

Language: Английский

Citations

62
Direct Photocatalytic Synthesis of Acetic Acid from Methane and CO at Ambient Temperature Using Water as Oxidant DOI
Chunyang Dong,

Maya Marinova,

Karima Ben Tayeb

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(2), P. 1185 - 1193

Published: Jan. 2, 2023

Direct functionalization of methane selectively to value-added chemicals is still one the main challenges in modern science. Acetic acid an important industrial chemical produced nowadays by expensive and environmentally unfriendly carbonylation methanol using homogeneous catalysts. Here, we report a new photocatalytic reaction route synthesize acetic from CH4 CO at room temperature water as sole external oxygen source. The optimized photocatalyst consists TiO2 support ammonium phosphotungstic polyoxometalate (NPW) clusters anchored with isolated Pt single atoms (Pt1). It enables stable synthesis 5.7 mmol·L–1 solution 60 h selectivity over 90% 66% on liquid-phase carbon basis, respectively, production 99 mol per Pt. Combined isotopic situ spectroscopy investigation suggests that proceeds via oxidative Pt1 sites, activation facilitated water-derived hydroxyl radicals.

Language: Английский

Citations

56
Enhanced photocatalytic degradation of toluene on surface C- and CN-modified TiO2 microspheres DOI
Da Wang,

Haole Tian,

Jiaxin Zhu

et al.

Applied Surface Science, Journal Year: 2024, Volume and Issue: 673, P. 160862 - 160862

Published: July 30, 2024

Language: Английский

Citations

55
Light-driven flow synthesis of acetic acid from methane with chemical looping DOI Creative Commons
Wenqing Zhang, Dawei Xi, Yihong Chen

et al.

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

Published: May 26, 2023

Oxidative carbonylation of methane is an appealing approach to the synthesis acetic acid but limited by demand for additional reagents. Here, we report a direct CH3COOH solely from CH4 via photochemical conversion without This made possible through construction PdO/Pd-WO3 heterointerface nanocomposite containing active sites activation and C-C coupling. In situ characterizations reveal that dissociated into methyl groups on Pd while oxygen PdO responsible carbonyl formation. The cascade reaction between generates acetyl precursor which subsequently converted CH3COOH. Remarkably, production rate 1.5 mmol gPd-1 h-1 selectivity 91.6% toward achieved in flow reactor. work provides insights intermediate control material design, opens avenue oxygenates.

Language: Английский

Citations

52