Nature Communications
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2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Wei Fen,Zhao Jiwu,Liu Yu-Chun,Hsu Yung-Hsi,Hung Sung-Fu,Fu Junwen,Liu Kunlong,Lin Wei,Yu Zhiyang,Tan Li,Lu Xue Feng,Feng Chengyang,Zhang Huabin,Wang Sibo
Lattice oxygen-mediated photocatalytic ethane dehydrogenation represents a sustainable strategy for ethylene production, yet achieving a balance between high productivity, selectivity, and durability remains challenging. Here, we report a defective NiO-300 catalyst, where precisely engineered Ni vacancies activate lattice oxygen by weakening Ni–O bond and improving lattice oxygen mobility. This promotes efficient ethane activation and C–H bonds cleavage through photoinduced hole capture, intensifying ethane dehydrogenation via a light-boosted Mars-van Krevelen mechanism. The NiO-300 catalyst manifests a high ethylene yield of 604.5 μmol g −1 h −1 with 100% selectivity and stability over 200 cycles. In situ spectroscopic and theoretical studies elucidate the generation of active oxygen species, the evolution of Ni coordination, the formation of key intermediates, and the underlying photocatalytic mechanism. Our findings highlight cation vacancy engineering as a powerful tactic to fully activate lattice oxygen for solar-driven alkene production from alkane dehydrogenation over oxide photocatalysts.
研究领域:
催化
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材料科学
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化学工程
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物理化学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kaiting Chen,Qingwei Li,Xinyu Han,Cheng Rao,Xiangguang Yang,Yibo Zhang
Developing efficient low-temperature selective catalytic reduction (CO-SCR) catalysts remains a key challenge in reducing nitrogen oxide (NOx) emissions. Here, we report a photothermal-enhanced Rh–Mn/CoAlOx heterostructure catalyst that achieves excellent NO conversion (more than 90% at 140 °C) and N2 selectivity (>80%) under visible to infrared light irradiation. By integration of highly dispersed Rh units with Mn clusters onto a hydrotalcite-derived CoAlOx support, the catalyst exhibits synergistic light absorption and dynamic lattice oxygen migration capabilities. Through combined analysis using in situ DRIFTS, XAFS, XPS, EPR, and other techniques, we reveal that Mn doping induces numerous oxygen vacancies and promotes electron transfer between Rh and Mn, facilitating lattice oxygen activation via a mechanism similar to the Mars-van Krevelen mechanism. Light exposure reduces the activation energy and, according to Arrhenius analysis and NO-TPD results, accelerates the decomposition of nitrate intermediates and enhances the conversion rate of nitrous oxide to N2. Density functional theory (DFT) calculations confirm that N2O is more likely to be generated at the Rh–Mn interface, demonstrating its enhanced low-temperature activation ability for NO. This study innovatively enhances the catalytic performance of CO-SCR using light, providing a sustainable method for reducing low-energy NOx emissions.
研究领域:
催化
·
环境化学
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材料科学
·
物理化学
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纳米技术
·
化学反应工程
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产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
Junjie Jiang,Yang Zou,Xue Li,Yongqi Zhao,Ziwei Zhao,Xiaolong Liu,Tingyu Zhu
Noble metal catalysts exhibit high efficiency and stability in CO removal, but their high loading of noble metals led to elevated costs, limiting industrial applications. This study selected three representative noble metals (Pt, Au, Ru) to investigate the CO reaction mechanisms on low-loading noble metal catalysts and the effects of SO2/H2O on CO oxidation. Catalysts with 0.1 wt% metal loading were synthesized via the impregnation method using conventional TiO2 as the support, denoted as 0.1Pt/Ti, 0.1Au/Ti and 0.1Ru/Ti. Among them, 0.1Pt/Ti achieved complete CO conversion at 270 °C and maintained 100% conversion over 46 h of continuous operation at 250 °C in the presence of SO2 and H2O. In situ DRIFTS indicated that the CO reaction over all catalysts followed the Mars–van Krevelen (MvK) mechanism. However, both Langmuir–Hinshelwood (L–H) and MvK pathways coexisted on 0.1Pt/Ti, with the L–H mechanism being dominant. DFT calculations revealed that CO also exhibited a higher adsorption preference for the 0.1Pt/Ti catalyst, which was identified as the primary reason for its superior performance.
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高影响因子
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