JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yunshuo Zhu,Lili Guan,Xiwen Song,Yarong Huang,Ming Li,Qingxian Zhang,Ruihua Guo
Strict control of carbon emissions is crucial for expediting the achievement of carbon neutrality. However, the current CO 2 RR electrocatalytic exhibits numerous shortcomings that impede the enhancement of catalytic activity. Issues such as lengthy catalyst preparation times, and high levels of precious metal content. Additionally, the aggregation of ultrafine nanoparticles contributes to a rapid deterioration in catalytic performance. Herein, a Joule-heating method is efficiently utilized to synthesize heterostructures nano-catalysts for CO 2 electroreduction on carbon cloth substrates. This method takes advantage of the thermoelectric coupling of the carbon cloth to achieve carbothermal reduction, while also regulating phase composition and introduction of oxygen vacancies. The Cu-CeO 2 /TiO 2 /CC catalyst synthesized in this method showed a current density in CO 2 of −32 mA·cm −2 at −1.0 V (vs. RHE). Notably, this catalyst demonstrated high CO selectivity and Faraday efficiency (FE CO ) of up to 82.5 % at a low potential of −0.3 V (vs. RHE). Optimal electrochemical performance is achieved at a power of 40 W. The ultra-fast temperature change process prevented the agglomeration of catalyst particles and facilitated the construction of a stable heterogeneous interface with a high oxygen vacancy concentration. In conclusion, this study presents a promising approach, particularly for the rapid preparation of low-cost, highly selective non-precious metal electrocatalysts.
研究领域:
材料科学
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环境科学
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电化学
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DOI
高影响因子
ChemSusChem
·
2026
·Vol. 19
·期 3
·e202502450
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IF 5.9
Mengmeng Jin,Yaolei Zhao,Weiting Li,Tiantian Xu,Jiazuo Wei,Jingjun Liu
2,5-Bis(hydroxymethyl)furan (BHMF) is a promising intermediate for the synthesis of pharmaceuticals and crown ethers, whereas achieving a high reaction rate in the hydrogenation of 5-hydroxymethylfurfural (5-HMF) to form BHMF remains challenge. In this work, a series of Cu/CeO 2 –x catalysts ( x denotes H, Air, Ar) were synthesized by calcination under different atmospheres (10% H 2 /Ar, Air, Ar) and evaluated for the 5-HMF hydrogenation to BHMF. Cu/CeO 2 –Ar exhibited a superior reaction rate of 26.8 mmol·g cat −1 ·h −1 and BHMF yield of 99.1% under the condition (180°C, 5 h, 1 MPa H 2 ), significantly outperforming Cu/CeO 2 –H and Cu/CeO 2 –Air. The characterizations reveal that the calcination in the oxygen-deficient argon atmosphere led to high Cu dispersion and minimized Cu particle size in the Cu/CeO 2 –Ar. These properties resulted in the abundant Cu + –O V –Ce 3+ sites and increased Cu 0 number. In situ Fourier transform infrared spectroscopy analysis elucidates the distinct roles of these active sites. Cu + sites are responsible for perpendicular adsorption of the 5-HMF carbonyl group, and Cu 0 sites drive efficient H 2 dissociation. In contrast, the O V –Ce 3+ sites do not adsorb 5-HMF and H 2 . The close synergy between numerous Cu 0 sites and abundant Cu + sites in the Cu/CeO 2 –Ar accelerates the process of 5-HMF hydrogenation to BHMF. Graphical The oxygen-deficient argon atmosphere led to high dispersion and small particle size of Cu in Cu/CeO 2 –Ar. These properties resulted in the abundant Cu + sites for the adsorption of CO from 5-HMF and the numerous Cu 0 sites to efficiently dissociate H 2 , synergistically boosting catalytic reaction rate to 26.8 mmol·g cat -1 ·h -1 .
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DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2018
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IF 4.521
Zihao Zhang,Changxue Wang,Xin Gou,Hao Chen,Kequan Chen,Xiuyang Lu,Pingkai Ouyang,Jie Fu
A series of Cu-based catalysts with different supports were synthesized and studied for the in situ hydrogenation of 5-hydroxymethylfurfural (5-HMF) to dimethylfuran (DMF) using methanol as an economical hydrogen donor. The structures and properties of the four catalysts (Cu/Al 2 O 3 , Cu/ZnO, Cu/ZrO 2 , and Cu/CeO 2 ) were characterized using X-ray diffraction (XRD), temperature-programmed reduction (H 2 -TPR), and temperature-programmed desorption of ammonia (NH 3 -TPD). The experimental results showed that the use of different supports for the Cu-based catalysts significantly influenced their activity for both H 2 production from methanol and hydrogenation of 5-HMF. The catalyst Cu/Al 2 O 3 showed the best catalytic activity, which can be attributed to the highest activity for the in situ H 2 production from methanol, smallest Cu crystallite size, and strongest acidity. The effects of the substrate concentration, catalyst loading, and reaction temperature and time on the in situ hydrogenation of 5-HMF were systematically investigated to determine the optimum reaction conditions.
研究领域:
催化
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化学工程
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材料科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Yudong Zhang,Long Liang,Ziyang Chen,Jinjun Wen,Wen Zhong,Sibei Zou,Mingli Fu,Limin Chen,Daiqi Ye
Self-assembled CeO 2 with 3D hollow nanosphere, nanoparticle and nanocube morphologies were prepared and used to support Cu particles. The obtained samples (denoted as Cu/CeO 2 -hs, Cu/CeO 2 -np and Cu/CeO 2 -nc, respectively) were tested for the reverse water-gas shift (RWGS) reaction. Under the reaction conditions, V (H 2 ): V (CO 2 ) = 3:1 and weight hourly space velocity (WHSV) = 300,000 mL g −1 h −1 , the Cu/CeO 2 -hs sample exhibited the best catalytic performance among the as-prepared catalysts. In order to reveal the key factors affecting the catalytic performance, the physicochemical properties of the catalysts were analyzed by XRD, BET, SEM, TEM, H 2 -TPR, quasi in-situ XPS and in situ UV-Raman techniques. The results point out that the particle size of Cu is not the rate-determining factor while the amount of surface oxygen vacancies is highly correlated with the catalytic reaction rate. In situ UV-Raman and in situ DRIFTS experiments indicate the formation of bidentate carbonate and formate species on oxygen vacancy sites which is thought to be the key intermediates for the RWGS reaction. These findings unravel the crucial roles of surface oxygen vacancies on CO 2 adsorption and activation and also highlight a feasible way for the design of highly efficient catalysts for the important RWGS reaction in chemical industry.
研究领域:
催化化学
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材料科学
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DOI
高影响因子