ChemCatChem
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2025
·
IF 3.9
Pengwei Deng,Haoran Wu,Huayu Wei,Zixu Yang,Jing Xu,Minghui Zhu
Graphical A modified synthesis method on Cu mesh simplifies and enhances the catalyst preparation process and efficiency at a much lower cost. The synergistic interplay between Co and Cu species is further investigated during the 5-hydroxymethylfurfural oxidation reaction. The Co-doped Cu mesh catalyst's scalability, cost-effectiveness, and robust performance underscore its potential for industrial applications in 5-hydroxymethylfurfural electrooxidation. The growing demand for sustainable alternatives to fossil-derived chemicals has spurred significant interest in biomass valorization, with 5-hydroxymethylfurfural (HMF) emerging as a key platform molecule. In this study, an electrochemical synthesis strategy was employed to synthesize a bimetallic Co-doped Cu mesh catalyst for the HMF oxidation reaction. It exhibited remarkable electrooxidation activity during a 3-h reaction at 1.6 V versus RHE with 83.2% HMF conversion, 99.4% 2,5-furandicarboxylic acid (FDCA) selectivity, and 87.7% Faraday efficiency. X-ray diffraction, in situ surface-enhanced Raman spectroscopy, and X-ray photoelectron spectroscopy revealed that the modified Cu mesh catalyst introduced more Co 3 O 4 species. Additionally, in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy elucidated that Cu species on the Co-doped Cu mesh can adsorb *OH and couple with organic molecules during the reaction process. Cu─Co dual active sites enhance the selective electrochemical oxidation of HMF toward FDCA.
研究领域:
化学工程
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材料科学
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可再生资源
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Lingfang Kong,Yi Liu,Zhonggao Zhou,Zhichao He,Yun Bai,Guohai Xu,Yunxiang Pan,Hongyu Zhen,Yiwang Chen
The conversion of carbon dioxide (CO 2 ) and propargylamines to 2-oxazolidinones is an essential reaction in industry, but efficiently activating both feedstocks remains a huge challenge for majority of catalysts. Herein, we developed a long-term stable copper catalyst, co-coordinated with sugar acetates (acetylglucose, AcGlu) and 2-methyl-imidazolium (Im-Cu A ). This catalyst features multi-active site, enabling it to efficiently capture and activate CO 2 , activate propargylamines, and stabilize the catalyst species simultaneously. As expected, 2-oxazolidinone was synthesized by this cyclization reaction with an exciting turnover frequency of 880 h −1 , which is around 180 times higher than that of CuCl 2 . Moreover, the catalytic activity of Im-Cu A did not decrease even after 20 replicates, which is exceptionally rare for homogeneous catalysts. Density functional theory calculations indicate that the electron-donating AcGlu and 2-methyl-imidazolium units facilitate electrons transport from Im-Cu A to CO 2 . Moreover, the high electron density of AcGlu and 2-methyl-imidazolium groups is believed to play a crucial role in the long-term stability across various temperatures and excellent catalytic performance of Im-Cu A . This represents a significant advancement in the development of a highly stable copper catalyst with multi-active site that effectively activates all reaction substrates. This strategy could improve the development of metal catalysts with sustained superior performance for CO 2 conversion.
研究领域:
化学催化
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材料科学
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环境科学
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DOI
高影响因子
Molecular Catalysis
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2017
·
IF 0
Hao Chen,Houhang Ruan,Xilei Lu,Jie Fu,Timothy Langrish,Xiuyang Lu
Catalytic transfer hydrogenation of furfural to furfuryl alcohol is considered to be a very important industrial process. In this work, non-noble Cu supported on MgO-Al 2 O 3 catalysts have been prepared by co-precipitation and have shown excellent catalytic performance for conversion of furfural to furfuryl alcohol in near-critical iso-propanol. The effects of the Cu state (reduction degree and dispersion) and loading in Cu/MgO-Al 2 O 3 , acidity of catalysts have been investigated by X-ray diffraction (XRD), coupled plasma optical emission spectrometry (ICP-OES), N 2 adsorption and desorption (N 2 -BET) and temperature-programmed desorption of ammonia (NH 3 -TPD), which have led to high activity for producing furfuryl alcohol. The results have shown that the selectivity of furfuryl alcohol has been influenced by the Cu state, Lewis acidity, reaction temperature and reaction time. The mechanisms, Lewis acid- and metal mediated hydrogenation, have shown that a desirable balance of Cu loading and Lewis acidity of catalyst has influenced the activity significantly. Almost 100% furfural conversion, with 89.3% furfuryl alcohol yield has been obtained. Cycling tests have shown that the prepared catalysts have been stable, where recycling the catalysts at least four times has not shown any reduction in activity.
研究领域:
化学工程
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催化材料
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DOI
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 19
·5414-5426
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IF 9.405
Yu Ding,Jingxia Tian,Wei Chen,Yejun Guan,Hao Xu,Xiaohong Li,Haihong Wu,Peng Wu
Copper-based catalysts, with highly dispersed and stabilized Cu nanoparticles, intensified mass transfer and a well-balanced Cu0/Cu+ ratio at low Cu loadings, are highly desirable for the selective hydrogenation of ethylene carbonate to ethylene glycol and methanol, an efficient indirect route of CO2 utilization. A hierarchically core/shell-structured Silicalite-1@Cu composite was developed via a base-assisted chemoselective host–guest interaction between the silicon species of MFI-type Silicalite-1 and external Cu salt source. In situ generated mesoporosity and strong Cu–silicate interaction made the uniform Cu NPs firmly immobilized and highly dispersed outside the core S-1 crystals. The S-1@Cu hybrid possessed the co-existing Cu0/Cu+ active species with a suitable ratio, and served as a highly active, selective and robust catalyst for selective ethylene carbonate hydrogenation, providing a lifetime >350 h together with >99% ethylene carbonate conversion, >99% ethylene glycol yield, and more importantly 93% methanol yield at a relatively low Cu loading of 21.4 wt%.
研究领域:
化学工程
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催化材料
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能源化学
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Hongge Cui,Xinli Tong,Linhao Yu,Ming Zhang,Yongtao Yan,Xuli Zhuang
An efficient tandem process for the oxidative condensation of furfural (FUR) with ethanol catalyzed by the copper/azodicarboxylate system has been developed. Firstly, the hydrogen transferring between FUR and ethanol is investigated under the nitrogen atmosphere by combining the azodicarboxylate and alkali carbonates, in which the main products are furfuryl alcohol and furan-2-acrolein. In the following, the cuprous halides and molecular oxygen are supplemented into the reaction system in order to improve the yield of furan-2-acrolein; therein, it is found that furfuryl alcohol is further oxidized and the selectivity of furan-2-acrolein is obviously elevated when CuI and o-phenanthroline (Phen) are used as the co-catalysts. Under optimal reaction conditions, 82.5% conversion of FUR with 87.7% selectivity of furan-2-acrolein is obtained with the assistance of diethyl azodicarboxylate (DEAD) and potassium carbonate. At last, a possible catalytic mechanism is proposed for the oxidative condensation reaction between FUR and ethanol in the presence of O 2 .
研究领域:
化学
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生物质转化
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产品关联
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 2
·450
·
IF 3.9
Muhammad Naeem Younis,Zhiheng Ren,Chunshan Li,Erqiang Wang,Jie Li
The advancing effects of various alkali and alkaline earth metals (inclusive of K, Ca, and Sr) modified Cu/SiO2catalysts, prepared with a modified precipitation-gel method, were investigated for the production of ethanol via hydrogenation of methyl acetate. Our results showed that Sr-doped catalysts exhibited the best and most consistent results during catalytic tests. A series of techniques, including X-ray diffraction technique, Raman spectroscopy, N2adsorption/desorption, N2O titration method, FTIR spectroscopy, and H2temperature, programmed desorption and reduction (TPD and TPR), and X-ray Photoelectron Spectroscopy, which was used to check the detailed characterization of Sr modification in the catalyst and its structural impacts on the properties of the catalyst. These results demonstrated that the addition of 5%Sr could strengthen the intrinsic stability of the catalyst by formulating the appropriate ratio of Cu+/(Cu0+ Cu+) to facilitate catalytic outcome improvement. The addition of 5%Sr-30%Cu/SiO2under the most favorable conditions, resulting in the peak conversion of MA (95%) and ethanol selectivity (96%), indicates its magnificent catalytic stabilizing effects. Furthermore, the best performing catalyst was compared and tested under various conditions (LHSV and temperatures) and a 300 h long life run.Keywords:hydrogenation;methyl acetate;ethanol;strontium
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 36
·17072-17079
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IF 3.3
Hongmei Xie,Guozhi Zhu,Dawei Ye,Weiquan Cai,Junjie Zhang,Kangping Huang,Yuliang Mai,Bing Liao,Jiazhi Chen
Catechyl lignin (C-lignin) is a unique and attractive natural biopolymer used as raw material for the production of chemicals and materials due to its homogeneous linear aromatic structure. Tung nutshells, an important component of industrial solid waste, are rich in C/G-type Lignin. Herein, for the first time, we report that the catalytic oxidation strategy is effective for the conversion of Tung nutshell lignin to value-added C/G-type aromatic monomers using the commercially available CuCl2 catalyst. The reaction conditions, including solvent, temperature, and catalyst dosage, were comprehensively investigated. The optimal yield of 60.8 mg g−1 (or 12.9 wt% Klason lignin) C/G-type aromatic aldehydes and acids was obtained using the CuCl2 catalyst in the CH3CN/H2O (8/2, v/v) solvent mixture at 190 °C for 4 h. The C-type aromatic monomers were formed with an yield of 7.7 mg g−1 (or 1.6 wt%) in the initial 0.2 h and gradually decreased as the reaction progressed. The less amount of C-type lignin-derived aromatic monomers can be attributed to their lower thermal stability under oxidative conditions. The structural evolution study of lignin by GPC and HSQC NMR reveals that the C/G units are effectively depolymerized and transformed into aromatic aldehydes and acids by the CuCl2/CH3CN/H2O catalytic oxidative system.
研究领域:
化学工程
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生物质能
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有机化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Xiangxue Zhang,Nina Fei,Qianhong Wang,Ali Raza Khan,Wenyao Chen,Gang Qian,Jing Zhang,De Chen,Xuezhi Duan,Xing-Gui Zhou,Weikang Yuan
Oxygen vacancy regulation in metal catalysts has emerged as a crucial strategy for efficiently degrading volatile organic compounds (VOCs), while the acquisition of kinetics and mechanistic insights into the oxygen vacancy roles remains highly desirable yet challenging. Herein, we conduct a combined kinetics and mechanistic investigation into the oxygen vacancy effects of Cu catalysts on toluene oxidation. Cu catalysts with varying oxygen vacancy contents are prepared using three representative metal oxide supports, including reducible ZrO2 with strong oxygen storage capacity, reducible ZnO, and unreducible Al2O3. The toluene oxidation as well as CO oxidation are tested for these catalysts, revealing the superior catalytic activity of Cu/ZrO2 catalyst. Multiple charactrizations demonstrate that the strong reducibility and abundance of oxygen vacancies within the Cu/ZrO2 catalyst are the key factors for these reactions. A redox-based kinetics strategy is further applied to decouple the reduction and oxidation steps, thus affording a rate diagram to elucidate the promotional effects of oxygen vacancies on toluene decomposition. Additionally, in-situ DRIFTS study unveils the reaction pathway, showing the transformation from toluene to benzyl alcohol, benzaldehyde, benzoate, phenol, anhydride, carbonate, and ultimately to CO2. As a result, the oxygen vacancy-tuned rate-relevant step is disclosed, shifting from C-H bond cleavage for the Cu/Al2O3 catalyst with limited oxygen vacancies to the C=O and C=C bond cleavage for the Cu/ZnO and Cu/ZrO2 catalysts with more oxygen vacancies. The kinetics and mechanistic insights gained here would help guide the design of highly efficient oxidative catalysts by tuning the oxygen vacancies of support.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2017
·Vol. 32
·期 1
·e3946
·
IF 2.319
Xingquan Xiong,Zhongke Tang,Zhaohong Sun,Xiaoqing Meng,Sida Song,Zhilong Quan
An eco-efficient, green, and multi-gram procedure is presented for one-pot multicomponent synthesis of N -substituted 1,2,3-triazoles by using waste fishbone powders supported CuBr (FBPs-CuBr) as catalyst. FBPs-CuBr is found to be an efficient heterogeneous catalyst and a series of 1,2,3-triazoles are obtained in moderate to excellent yields in water under MW irradiation (70–98%). It can be separated conveniently by a simple filtration and reused at least seven consecutive runs with a slight drop in the product yields. Furthermore, the desired product still could be obtained in 80% yield when the scale of the reaction was increased to 40.0 mmol.
研究领域:
有机化学
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绿色化学
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催化材料
✓ 已验证
DOI
高影响因子
Nature Communications
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2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Yi,Wang Shuo,Fu Yunfan,Sang Jiaqi,Wei Pengfei,Li Rongtan,Gao Dunfeng,Wang Guoxiong,Bao Xinhe
Renewable energy-driven electrocatalytic nitrate reduction reaction presents a low-carbon and sustainable route for ammonia synthesis under mild conditions. Yet, the practical application of this process is currently hindered by unsatisfactory electrocatalytic activity and long-term stability. Herein we achieve high-rate ammonia electrosynthesis using a stable amorphous/crystalline dual-phase Cu catalyst. The ammonia partial current density and formation rate reach 3.33 ± 0.005 A cm −2 and 15.5 ± 0.02 mmol h −1 cm −2 at a low cell voltage of 2.6 ± 0.01 V, respectively. Remarkably, the dual-phase Cu catalyst can maintain stable ammonia production with a Faradaic efficiency of around 90% at a high current density of 1.5 A cm −2 for up to 300 h. A scale-up demonstration with an electrode size of 100 cm 2 achieves an ammonia formation rate as high as 11.9 ± 0.5 g h −1 at a total current of 160 A. The impressive electrocatalytic performance is ascribed to the presence of stable amorphous Cu domains which promote the adsorption and hydrogenation of nitrogen-containing intermediates, thus improving reaction kinetics for ammonia formation. This work underscores the importance of stabilizing metastable amorphous structures for improving electrocatalytic reactivity and long-term stability.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Heba Emam,Rashid Al Hajri,Nazir Ahmad,Fatma M. Elantabli,M. El-Rabiei,Abdelwahab Hassan,Mohammed Al Abri,Hussein A. Younus
The quest for an efficient and sustainable electrocatalyst for hydrogen evolution reaction (HER) using earth-abundant elements is crucial for cost-effective and environmentally friendly hydrogen production. While many catalysts show good activity and stability in strongly basic conditions, fewer materials are effective under neutral conditions, which are more practical for electrolyzer operations. This study introduces a dinuclear copper catalyst, [Cu 2 (μ-OH) (μ-NO 3 ) (L) 2 ], where L is the Schiff base ligand derived from salicylaldehyde and histidine amino acid (Complex 1 ), for HER in both aqueous and non-aqueous environments. In non-aqueous conditions, with acetic acid as a proton source, the catalyst exhibits outstanding HER performance, achieving an overpotential of 170 mV. At an acid concentration of 0.086 M, it achieves a catalytic current of ∼17.5 mA cm −2 at an overpotential of 0.52 V. Remarkably, in fully aqueous neutral conditions, Complex 1 reaches a significant current density with an i c /i p ratio of ∼82 at a scan rate of 1.0 V s −1 , and an apparent rate constant ( k obs ) for electrocatalytic HER of ∼13,200 s −1 . The catalyst also shows excellent activity in 0.1 M H 3 PO 4 , with low overpotentials of ∼150 mV at 2.0 mA cm⁻ 2 and 270 mV at 10.0 mA cm⁻ 2 . In controlled potential electrolysis (CPE), the catalyst maintains stable catalytic currents of 25 mA cm⁻ 2 and 75 mA cm⁻ 2 for 18–28 h at a potential of 0.590 V vs. RHE in neutral and acidic conditions, respectively, without noticeable decrease in catalytic current. Detailed characterizations confirm the molecular integrity of the catalyst and its predominantly homogeneous catalytic mechanism.
研究领域:
化学
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材料科学
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能源科学
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产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 9
·1049
·
IF 4.501
Yan Hao,Dajie Zhao,Wen Liu,Min Zhang,Yixiao Lou,Zhenzhen Wang,Qinghu Tang,Jinghe Yang
Selective dehydrogenation of ethanol to acetaldehyde has been considered as an important pathway to produce acetaldehyde due to the atom economy and easy separation of acetaldehyde and hydrogen. Copper catalysts have attracted much attention due to the high activity of Cu species in O-H and C-H bonds oxidative cleavage, and low process cost; however, the size of the Cu nanoparticle is difficult to control since it is easily suffers from metal sintering at high temperatures. In this work, the Cu/KIT-6 catalyst exhibited an ultra-high metal dispersion of 62.3% prepared by an electrostatic adsorption method, due to the advantages of the confinement effect of mesoporous nanostructures and the protective effect of ammonia water on Cu nanoparticles. The existence of an oxidation atmosphere had a significant effect on the valence state of copper species and enhancing moderate acid sites. The catalyst treated by reduction and then oxidation possessed a moderate/weak acid site ratio of ~0.42 and a suitable proportion of Cu+/Cu0ratio of ~0.53, which conceivably rendered its superior ethanol conversion of 96.8% and full acetaldehyde selectivity at 250 °C. The catalyst also maintained a high selectivity of >99% to acetaldehyde upon time-on-stream of 288 h.Keywords:copper;ethanol dehydrogenation;mesoporous silica
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）