Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Song Hui,Sun Kai,Huang Hengming,Ning Shangbo,Wang Shengyao,Wang Zhuan,Weng Yuxiang,Cui Yi,Li Yifan,Wang Xu-sheng,Wang Defa,Liu Lequan,Wang Zhou-jun,Ye Jinhua
The direct photocatalytic oxidation of methane to value-added chemicals has garnered considerable interest in recent years. However, achieving high productivity while maintaining high selectivity at an appreciable methane conversion rate remains a formidable challenge. Here, we present photochemically-triggered and photothermally-enhanced oxidative coupling of methane to multi-carbon C 2+ alkanes over an Au and CeO 2 nanoparticle-decorated ZnO photocatalyst, which exhibits a record-breaking C 2+ production rate of 17,260 μmol g −1 h −1 with ~90% C 2+ selectivity under wide-spectrum light irradiation without a secondary source of heating. Comprehensive characterizations and computational studies reveal that CH 4 activation is a photochemical reaction initiated by ultraviolet light-excited ZnO, and the introduction of CeO 2 substantially enhances the activation of CH 4 and O 2 due to the cooperative interaction between Au and CeO 2 . Concurrently, Au nanoparticles capture visible and near-infrared light to generate localized heating, which greatly promotes the subsequent desorption of produced methyl radical for C–C coupling prior to undergoing further undesired overoxidation.
研究领域:
化学工程
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Mingrui Wang,Peng Wang,Guanghui Zhang,Zening Cheng,Mengmeng Zhang,Yulong Liu,Rongtan Li,Jie Zhu,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Thomas P. Senftle,Xiaowa Nie,Qiang Fu,Chunshan Song,Xinwen Guo
The decomposition of cobalt carbide (Co 2 C) to metallic cobalt in CO 2 hydrogenation results in a notable drop in the selectivity of valued C 2+ products, and the stabilization of Co 2 C remains a grand challenge. Here, we report an in situ synthesized K-Co 2 C catalyst, and the selectivity of C 2+ hydrocarbons in CO 2 hydrogenation achieves 67.3% at 300°C, 3.0 MPa. Experimental and theoretical results elucidate that CoO transforms to Co 2 C in the reaction, while the stabilization of Co 2 C is dependent on the reaction atmosphere and the K promoter. During the carburization, the K promoter and H 2 O jointly assist in the formation of surface C * species via the carboxylate intermediate, while the adsorption of C * on CoO is enhanced by the K promoter. The lifetime of the K-Co 2 C is further prolonged from 35 hours to over 200 hours by co-feeding H 2 O. This work provides a fundamental understanding toward the role of H 2 O in Co 2 C chemistry, as well as the potential of extending its application in other reactions.
研究领域:
催化化学
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化学工程
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材料科学
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可持续能源
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多相催化
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DOI
高影响因子
ACS Catalysis
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2025
·
IF 13.1
Weina Yang,Yachao Wang,Yaxiong Wei,Guofeng Zhao,Weixin Huang,Cong Fu
Photocatalytic oxidative coupling of methane (OCM) offers a sustainable pathway for direct conversion of methane into value-added hydrocarbons, yet faces persistent challenges in balancing efficient methane activation with suppression of overoxidation. Here, we present a TiO2-based photocatalyst decorated with highly dispersed Ag–Co dual sites that achieves superior performance in continuous-flow OCM. The optimized AgCo–TiO2 system demonstrates a remarkable C2 hydrocarbon production rate of 1.7 mmol g–1 h–1 with 91% selectivity while maintaining stable operation for over 30 h. In situ spectroscopic analyses indicate that the introduced Co species induce mobile-charge imbalances, driving the directional transfer of photogenerated electrons and effectively suppressing electron–hole recombination. Coupled with Ag serving as a catalytic center, these effects synergistically enhance O2 activation, C–H bond cleavage, and selective C–C coupling, thereby contributing to the superior catalytic performance. This work provides valuable mechanistic insights into the photocatalytic OCM process, highlighting the pivotal role of precisely engineered charge transfer pathways in enabling efficient methane-to-C2 conversion.
研究领域:
光催化
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材料科学
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化学工程
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环境化学
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能量转换
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产品关联
DOI
高影响因子