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218 results on '"Qian, Qingli"'

6. Catalyst‐Green Solvent System for Highly Efficient Production of Carboxylic Acids from Light Oxygenates, CO2 and H2

Author

Wang, Yanyan, primary, Zhang, Yanru, additional, Wang, Ying, additional, Zhang, Longbo, additional, He, Jun, additional, Yu, Chenglong, additional, Li, Yang, additional, Zhang, Pei, additional, Ma, Jun, additional, Sun, Xiaofu, additional, Kang, Xinchen, additional, Zhen, Yuan, additional, Qian, Qingli, additional, and Han, Buxing, additional

Published
2024
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7. Highly Efficient Electrosynthesis of Glycine over an Atomically Dispersed Iron Catalyst

Author

Cheng, Yingying, primary, Liu, Shiqiang, additional, Jiao, Jiapeng, additional, Zhou, Meng, additional, Wang, Yiyong, additional, Xing, Xueqing, additional, Chen, Zhongjun, additional, Sun, Xiaofu, additional, Zhu, Qinggong, additional, Qian, Qingli, additional, Wang, Congyang, additional, Liu, Huizhen, additional, Liu, Zhimin, additional, Kang, Xinchen, additional, and Han, Buxing, additional

Published
2024
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9. Catalyst‐Green Solvent System for Highly Efficient Production of Carboxylic Acids from Light Oxygenates, CO2 and H2.

Author

Wang, Yanyan, Zhang, Yanru, Wang, Ying, Zhang, Longbo, He, Jun, Yu, Chenglong, Li, Yang, Zhang, Pei, Ma, Jun, Sun, Xiaofu, Kang, Xinchen, Zhen, Yuan, Qian, Qingli, and Han, Buxing

Subjects
CATALYTIC hydrogenation, HOMOGENEOUS catalysis, CARBON dioxide, EPOXY compounds, IONIC liquids, CARBOXYLIC acids
Abstract

Catalytic hydrogenation of carbon dioxide (CO2) for the preparation of higher carboxylic acids is attractive and promising. Herein, we demonstrate a general strategy for producing higher carboxylic acids via reaction of CO2 and H2 with light (C2~C4) oxygenates such as ketones, alcohols, polyols, ethers and epoxides. In a green solvent consisting of ionic liquid (1‐ethyl‐3‐methylimidazolium iodide) and water, the reaction can be efficiently accelerated by RhI3 catalyst and I2 promoter at 170 °C. Very high or remarkable yields of higher carboxylic acids were synthesized via C−C bond formation between the intermediates generated from the oxygenates and CO2. Detailed study indicated that the catalyst and the solvent had excellent synergistic effect for promoting the reaction. The strategy can effectively convert the bulk and inexpensive feedstocks to value‐added carboxylic acids, and therefore is promising for commercial application. [ABSTRACT FROM AUTHOR]

Published
2024
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11. Oxophilicity-Controlled CO2 Electroreduction to C2+ Alcohols over Lewis Acid Metal-Doped Cuδ+ Catalysts

Author

Zhang, Libing, primary, Feng, Jiaqi, additional, Wu, Limin, additional, Ma, Xiaodong, additional, Song, Xinning, additional, Jia, Shunhan, additional, Tan, Xingxing, additional, Jin, Xiangyuan, additional, Zhu, Qinggong, additional, Kang, Xinchen, additional, Ma, Jun, additional, Qian, Qingli, additional, Zheng, Lirong, additional, Sun, Xiaofu, additional, and Han, Buxing, additional

Published
2023
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14. Synthesis of Carboxylic Acids from Saccharides, CO2, and H2

Author

Li, Yang, primary, Wang, Ying, additional, Zhang, Yanru, additional, Wang, Zhenpeng, additional, Xiang, Junfeng, additional, Han, Juanjuan, additional, He, Jun, additional, Zhang, Longbo, additional, Wang, Yanyan, additional, Meng, Qinglei, additional, Qian, Qingli, additional, and Han, Buxing, additional

Published
2023
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16. Synergy of Cu/C3N4 Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid

Author

Yan, Xupeng, primary, Zhang, Menglu, additional, Chen, Yizhen, additional, Wu, Yahui, additional, Wu, Ruizhi, additional, Wan, Qiang, additional, Liu, Chunxiao, additional, Zheng, Tingting, additional, Feng, Rongjuan, additional, Zhang, Jing, additional, Chen, Chunjun, additional, Xia, Chuan, additional, Zhu, Qinggong, additional, Sun, Xiaofu, additional, Qian, Qingli, additional, and Han, Buxing, additional

Published
2023
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21. Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products.

Author

Feng, Jiaqi, Zhang, Libing, Liu, Shoujie, Xu, Liang, Ma, Xiaodong, Tan, Xingxing, Wu, Limin, Qian, Qingli, Wu, Tianbin, Zhang, Jianling, Sun, Xiaofu, and Han, Buxing

Subjects
ELECTROSYNTHESIS, COPPER, COUPLING reactions (Chemistry), PROTON transfer reactions, HYDROGEN, DOPING agents (Chemistry)
Abstract

Electrocatalytic CO2 reduction is a typical reaction involving two reactants (CO2 and H2O). However, the role of H2O dissociation, which provides active *H species to multiple protonation steps, is usually overlooked. Herein, we construct a dual-active sites catalyst comprising atomic Cu sites and Cu nanoparticles supported on N-doped carbon matrix. Efficient electrosynthesis of multi-carbon products is achieved with Faradaic efficiency approaching 75.4% with a partial current density of 289.2 mA cm−2 at −0.6 V. Experimental and theoretical studies reveal that Cu nanoparticles facilitate the C-C coupling step through *CHO dimerization, while the atomic Cu sites boost H2O dissociation to form *H. The generated *H migrate to Cu nanoparticles and modulate the *H coverage on Cu NPs, and thus promote *CO-to-*CHO. The dual-active sites effect of Cu single-sites and Cu nanoparticles gives rise to the catalytic performance. A dual-site catalyst consisting of Cu nanoparticles (NPs) and atomic Cu sites is designed. The atomic Cu boosts H2O dissociation for modulating the *H coverage on Cu NPs, improving the efficiency of CO2 electroreduction to multi-carbon products. [ABSTRACT FROM AUTHOR]

Published
2023
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25. Synergy of Cu/C3N4 Interface and Cu Nanoparticles Dual Catalytic Regions in Electrolysis of CO to Acetic Acid.

Author

Yan, Xupeng, Zhang, Menglu, Chen, Yizhen, Wu, Yahui, Wu, Ruizhi, Wan, Qiang, Liu, Chunxiao, Zheng, Tingting, Feng, Rongjuan, Zhang, Jing, Chen, Chunjun, Xia, Chuan, Zhu, Qinggong, Sun, Xiaofu, Qian, Qingli, and Han, Buxing

Subjects
COPPER, ACETIC acid, METALLIC surfaces, SOLID electrolytes, CARBON monoxide, DENSITY functional theory, ELECTROLYTIC reduction
Abstract

Electrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g‐C3N4) supported Cu nanoparticles (Cu−CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm−2 in CORR. In situ experimental and density functional theory calculation studies revealed that the Cu/C3N4 interface and metallic Cu surface synergistically promoted CORR into acetic acid. The generation of pivotal intermediate −*CHO is advantage around the Cu/C3N4 interface and migrated *CHO facilitates acetic acid generation on metallic Cu surface with promoted *CHO coverage. Moreover, continuous production of acetic acid aqueous solution was achieved in a porous solid electrolyte reactor, indicating the great potential of Cu−CN catalyst in the industrial application. [ABSTRACT FROM AUTHOR]

Published
2023
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27. Synthesis of Carboxylic Acids via Reaction of Ketones/Aldehydes with CO2and H2

Author

Zhang, Yanru, Zhang, Jingjing, Wang, Ying, Li, Yang, He, Jun, Wang, Yanyan, Zhang, Longbo, Wang, Zhenpeng, Qian, Qingli, and Han, Buxing

Abstract

Synthesis of basic C2+chemicals using CO2and H2is very promising. Herein, we present a protocol for the synthesis of different carboxylic acids by the reaction of ketones or aldehydes with CO2and H2. The catalytic system consisted of the IrCl3catalyst, LiI promoter, and acetic acid solvent. The yield can reach 52.9% based on the cyclohexanone substrate which can be derived from biomass. Various Cnketones and aldehydes could be used as a substrate in the reaction, where the corresponding Cn+1carboxylic acids were obtained. According to the mechanistic study, the reaction involved substrate conversion, reverse water–gas shift (RWGS) reaction, and carbonylation. This strategy provides an optional way of carboxylic acid production and CO2utilization.

Published
2023
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31. In Situ Periodic Regeneration of Catalyst during CO2 Electroreduction to C2+ Products.

Author

Xu, Liang, Ma, Xiaodong, Wu, Limin, Tan, Xingxing, Song, Xinning, Zhu, Qinggong, Chen, Chunjun, Qian, Qingli, Liu, Zhimin, Sun, Xiaofu, Liu, Shoujie, and Han, Buxing

Subjects
COUPLING reactions (Chemistry), CATALYSTS, CARBON offsetting, ELECTROLYTIC reduction, SURFACE structure, OXIDATION states, CATALYTIC cracking
Abstract

Developing electrocatalytic reactions with high‐efficiency can make important contributions to carbon neutrality. However, poor long‐term stability of catalysts is a bottleneck for its practical application. Herein, an "in situ periodic regeneration of catalyst (PR‐C)" strategy is proposed to give long‐term high efficiency of CO2 electroreduction to generate C2+ products over Cu catalyst by applying a positive potential pulse for a short time periodically in the halide‐containing electrolyte. The high Faradaic efficiency (81.2 %) and current density (22.6 mA cm−2) could be maintained completely at least 36 h, while the activity and selectivity decreased continuously without using the PR‐C method. Control experiments and operando characterization demonstrated that the surface structure and oxidation state of Cu could be recovered periodically by the PR‐C method, which was beneficial for CO2 activation and C−C coupling. [ABSTRACT FROM AUTHOR]

Published
2022
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37. The in situ study of surface species and structures of oxide-derived copper catalysts for electrochemical CO2 reduction

Author

Chen, Chunjun, primary, Yan, Xupeng, additional, Wu, Yahui, additional, Liu, Shoujie, additional, Sun, Xiaofu, additional, Zhu, Qinggong, additional, Feng, Rongjuan, additional, Wu, Tianbin, additional, Qian, Qingli, additional, Liu, Huizhen, additional, Zheng, Lirong, additional, Zhang, Jing, additional, and Han, Buxing, additional

Published
2021
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38. Synthesis of carboxylic acids via the hydrocarboxylation of alcohols with CO2 and H2.

Author

Zhang, Yanru, Wang, Ying, Qian, Qingli, Li, Yang, Asare Bediako, Bernard Baffour, Zhang, Jingjing, Yang, Junjuan, Li, Zhiyan, and Han, Buxing

Subjects
ALCOHOL, CARBOXYLIC acids, POLYOLS, IRIDIUM
Abstract

Production of higher carboxylic acids from CO2 and H2 is a novel and very attractive topic. Herein we present a protocol of synthesizing C3+ carboxylic acids via the reaction of alcohols with CO2 and H2. A catalytic system consisting of iridium(III) acetate and LiI could effectively accelerate this reaction. The reaction could occur at above 120 °C and the best result was obtained at 170 °C. The catalytic system could be applied to various alcohols (primary, secondary, and tertiary alcohols and polyols). The reaction mechanism was proposed based on systematic control experiments. [ABSTRACT FROM AUTHOR]

Published
2022
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40. In situ study of surface species and structure over Oxide-Derived Copper Catalysts for Electrochemical CO2 Reduction

Author

Chen, Chunjun, primary, Yan, Xupeng, additional, Wu, Yahui, additional, Liu, Shoujie, additional, Sun, Xiaofu, additional, Zhu, Qinggong, additional, Feng, Rongjuan, additional, Wu, Tianbin, additional, Qian, Qingli, additional, Liu, Huizhen, additional, Zheng, Lirong, additional, Zhang, Jing, additional, and Han, Buxing, additional

Published
2020
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41. Bromide promoted hydrogenation of CO2 to higher alcohols using Ru–Co homogeneous catalyst† †Electronic supplementary information (ESI) available: GC-MS and GC data. See DOI: 10.1039/c6sc01314g

Author

Cui, Meng, Qian, Qingli, He, Zhenhong, Zhang, Zhaofu, Ma, Jun, Wu, Tianbin, Yang, Guanying, and Han, Buxing

Subjects
Chemistry
Abstract

Higher alcohols can be synthesized efficiently by CO2 hydrogenation over Ru3(CO)12–Co4(CO)12 bimetallic catalyst with bis(triphenylphosphoranylidene)ammonium chloride (PPNCl) as the cocatalyst and LiBr as the promoter., Iodides are commonly used promoters in C2+OH synthesis from CO2/CO hydrogenation. Here we report the highly efficient synthesis of C2+OH from CO2 hydrogenation over a Ru3(CO)12–Co4(CO)12 bimetallic catalyst with bis(triphenylphosphoranylidene)ammonium chloride (PPNCl) as the cocatalyst and LiBr as the promoter. Methanol, ethanol, propanol and isobutanol were formed at milder conditions. The catalytic system had a much better overall performance than those of reported iodide promoted systems because PPNCl and LiBr cooperated very well in accelerating the reaction. LiBr enhanced the activity and PPNCl improved the selectivity, and thus both the activity and selectivity were very high when both of them were used simultaneously. In addition, the catalyst could be reused for at least five cycles without an obvious change of catalytic performance.

Published
2016

47. Synthesis of higher carboxylic acids via reaction of polyols with CO2and H2

Author

Asare Bediako, Bernard Baffour, Qian, Qingli, Wang, Ying, Zhang, Jingjing, Wang, Zhenpeng, Li, Shumu, Liu, Huizhen, Wu, Tianbin, Ge, Maofa, and Han, Buxing

Abstract

Synthesis of value-added chemicals from biomass-derived polyols and CO2is of great importance. Herein we report a strategy to produce higher carboxylic acids by the reaction of polyol, CO2, and H2. The reaction can be efficiently accelerated by Rh catalyst in a binary solvent of ionic liquid (1-butyl-3-methylimidazolium iodide) and water, where cheap and nontoxic I2was used as a promoter. The reaction can occur at above 100°C. At optimal conditions, the yield of the carboxylic acids was as high as 86.4%. The catalytic mechanism is proposed based on a series of control experiments. Interestingly, the polyol could be effectively transformed into olefin intermediate at metal-free and mild conditions, which was the key to the success of this strategy. The peculiar solvent effect was also favorable to the reaction. In addition, the catalytic system was adaptable to various polyol substrates.

Published
2022
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48. Highly selective hydrogenation of CO2 into C2+ alcohols by homogeneous catalysis† †Electronic supplementary information (ESI) available: Supplementary figures and tables. See DOI: 10.1039/c5sc02000j

Author

Qian, Qingli, Cui, Meng, He, Zhenhong, Wu, Congyi, Zhu, Qinggong, Zhang, Zhaofu, Ma, Jun, Yang, Guanying, Zhang, Jingjing, and Han, Buxing

Subjects
Chemistry, integumentary system, organic chemicals, bacteria, lipids (amino acids, peptides, and proteins), equipment and supplies
Abstract

Methanol, ethanol, propanol, 2-methyl propanol, butanol, and 2-methyl butanol were produced in homogeneous CO2 hydrogenation with a selectivity for C2+ alcohols of 96.4%., The hydrogenation of CO2 to produce alcohols with two or more carbons (C2+ alcohols) is of great importance, but is challenging. In this work, we found that a Ru3(CO)12/Rh2(CO)4Cl2–LiI system could catalyze the reaction effectively in 1,3-dimethyl-2-imidazolidinone (DMI) under mild conditions. Methanol, ethanol, propanol, 2-methyl propanol, butanol, and 2-methyl butanol were produced in the homogeneous catalytic reaction. The C2+ alcohols could be generated at 160 °C, which is the lowest temperature reported so far for producing C2+ alcohols via CO2 hydrogenation. The selectivity for the C2+ alcohols could be as high as 96.4% at the optimized conditions, which is higher than those reported in the literature. In addition, the catalytic system could be easily recycled. The route of the reaction for forming the C2+ alcohols was discussed on the basis of control experiments.

Published
2015

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