CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ning Liu,Na Lu,Kun Zhao,Pengxiao Liu,ZhuMei Sun,Jing Lu
The conversion of methane (CH 4 ) and carbon dioxide (CO 2 ) into high-value products under mild conditions is crucial for addressing the greenhouse effect and advancing C1 chemistry. In this study, Cu/ZnO catalysts were prepared through a one-step wet reduction process, and the catalytic conversion of CH 4 and CO 2 into acetic acid molecules (CH 3 COOH) was achieved via photon activation at ambient temperature. The yield of acetic acid was 411.6 μmol/Lg cat −1 h −1 with a selectivity of 89.5 % under optimal conditions (100 mWcm −2 light intensity, 25 ± 2 °C, 2 MPa pressure, and a 1:1 CH 4 :CO 2 volume ratio). Enhanced solubility of CH 4 in aqueous under increased pressure and temperature was observed to improve acetic acid production. Additionally, the catalytic mechanism involved surface chemisorption of CH 4 and CO 2 , facilitated by ZnO and Cu in the catalyst, leading to C-C coupling and subsequent acetic acid formation, driven by photogenerated electron-hole migration. This study provides a foundational understanding for the synthesis of value-added chemicals through CH 4 and CO 2 conversion via C-C coupling in mild environments.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2024
·
IF 5
Xueyang Ren,Jie Zheng,Jinxian Zhao,Jun Ren,Yanhong Quan
The one-step oxidative esterification of ethylene glycol (EG) is an effective and promising route for methyl glycolate (MG) synthesis, during which the development of efficient catalysts is critically crucial. Herein, Au/ZnO catalysts were prepared using impregnation (IM), colloidal-deposition (CD), deposition-precipitation (DP) and co-precipitation (CP) methods, respectively. The catalytic activities results revealed that the Au/ZnO-DP catalyst was far superior than the other three catalysts, achieving an EG conversion rate of 90.4% and a selectivity towards MG of 93.8%. Catalysts were systematically characterized by N2 adsorption-desorption, XRD, TEM, XPS, H2-TPR, EPR, O2-TPD and CO2-TPD. The results showed that the large number of Au-ZnO interfaces facilitated the adsorption and activation of O2. Moreover, it is found that the basic sites promoted the cleavage of O-H bonds in the EG molecules, and the acidic sites are responsible for the selectivity of MG. This work offers a simple strategy for design of gold catalysts in EG oxidative esterification.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 6
·4443-4457
·
IF 4.6
Junqi Zhang,Yongwang Li,Zhiwei Zhang,Zheng Wang,Jiaxing Zhang,Shuai Liu,Yang Qin,Bingxin Zhu,Tongxue Zhang,Hongyu Wang,Fumin Wang,Xubin Zhang
The development of simple, efficient and economical catalysts for the hydrogenation of biomass to produce high value-added chemicals is of great significance in solving the energy crisis. In this work, a series of non-precious metal catalysts (Cu–Al2O3–ZnO) with different defect sites were prepared by etching Devarda's alloy. Under optimized mild reaction conditions, the furfural conversion and furfuryl alcohol selectivity are both greater than 99.0%, and the catalyst has good reusability. Characterisation and experiments were used to investigate the activate species for hydrogenation reaction. It can be proved that the low-valent Cu species in the Cu–Al2O3–ZnO catalysts play an important role as adsorption and dissociation sites for H2. Different etching degrees and sample reduction temperatures of the alloy can be used to adjust the content of acidic sites such as Al2O3 and CuO, which have appropriate adsorption properties for furfural. ZnO promotes the dispersion of the Cu species and enhances the accessibility of the active sites. The etching method achieves the interaction between species to further enhance the stability and activity of the catalyst. The catalytic performance of the catalyst is very competitive and this study provides a new method for the efficient hydrogenation of furfural to furfuryl alcohol.
研究领域:
化学工程
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可再生能源
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of CO2 Utilization
·
2018
·
IF 5.503
Jiaxiong Liu,Dehua He
ZnWO 4 -ZnO catalysts with different W content were prepared by conventional hydrothermal and wet impregnation methods and applied in the direct synthesis of glycerol carbonate from CO 2 and glycerol. The crystallite structure, texture property, morphology, redox and acid-base properties and the surface chemical situation of the catalysts were characterized by XRD, BET, TEM, H 2 -TPR, NH 3 /CO 2 -TPD and XPS. The possible activation routes of CO 2 and glycerol were analyzed with DRIFTS and FTIR. ZnWO 4 -ZnO composite catalysts showed better catalytic performances with respect to ZnO in the carbonylation of glycerol with CO 2 . The improved activity of ZnWO 4 -ZnO catalysts was associated with the formation of ZnWO 4 , the interaction between ZnWO 4 and ZnO, and the enhanced moderate acidic property. DIRFTS results showed that chelating bidentate carbonate species was the main adsorption pattern for CO 2 on ZnO, while the introduction of W led to the bridged bidentate carbonate, which became the main adsorption pattern on ZnWO 4 -ZnO. As for the activation of glycerol, zinc glycerolate played an important role in the reaction process. Based on the reaction and characterization results, a plausible reaction route involved a seven-membered ring esters intermediate was suggested for the reaction of CO 2 and glycerol over ZnWO 4 -ZnO catalysts.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2020
·
IF 3.612
Pengbo Wang,Qian He,Hao Zhang,Qingdi Sun,Yujie Cheng,Tao Gan,Xiaohui He,Hongbing Ji
Several research studies have been conducted on N -formylation of amines using phenylsilane and CO 2 . However, most of these studies involved tedious processes of catalyst preparation or complex procedures. In the present study, we describe the use of a simple and commercially available ZnO catalyst for selective N -formylation of amines under mild condition. High-yielding N -formylation products with good recyclability and wide substrate scope were obtained, which can promote fine chemical synthesis and CO 2 capture.
研究领域:
有机化学
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催化化学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2017
·Vol. 122
·期 2
·1129-1143
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IF 1.264
Hou Miaomiao,Jiang Hong,Liu Yefei,Chen Rizhi
The work aims to investigate the role of initial water content in the glycerol hydrogenolysis to 1,2-propanediol over Cu–ZnO in depth by characterizing the fresh and spent catalysts in detail with ICP, XRD, XPS, EDS, HRTEM, N 2 sorption, N 2 O chemisorption, H 2 -TPD and NH 3 -TPD. The glycerol conversion and 1,2-propanediol selectivity gradually reduce simultaneously with increasing initial water content. At higher initial water content, more CuO are formed, bringing about a decrease in the 1,2-propanediol selectivity. The sizes of Cu and ZnO crystallites increase tremendously with increasing initial water content, lowering the active surface area and acidity. Furthermore, the surface Cu content reduces along with the increase of surface Zn content at higher initial water content. The two aspects make a decrease in the glycerol conversion. This work would aid the glycerol hydrogenolysis to 1,2-propanediol over Cu–ZnO with high catalytic efficiency.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guiming Xie,Xingyang Bai,Yi Man,Pengju Ren,Rongrong Jin,Runduo Zhang,Kostya (Ken) Ostrikov,Zhou-jun Wang,Qingyuan Yang
Innovative catalyst design and in-depth mechanism understanding are imperative for industrialization of CO 2 hydrogenation to methanol. Herein, Al-doped Cu/ZnO catalysts, Cu/Al-ZnO-x (x = 1/32, 1/16 and 1/8, denoting Al/Zn molar ratio), were creatively synthesized using MIL-53(Al) as Al sources and reactive templates. The Cu/Al-ZnO-1/16 catalyst exhibited the highest methanol production rate among the Cu/Al-ZnO-x catalysts, which was 1.93 times as active as the conventional Cu/Al-ZnO-1/16-C catalyst using Al(NO 3 ) 3 ·9H 2 O as Al source. Structural characterizations reveal that the use of MIL-53(Al) led to higher S BET , more uniform Al distribution, more abundant oxygen vacancies, more appropriate metal-support interactions and larger amount of medium basic sites. Mechanism studies demonstrate that Al doping would markedly induce oxygen vacancy formation on Cu-ZnO interfaces and thus significantly boost methanol synthesis activity. This work offers a facile approach to develop efficient methanol synthesis catalysts and provides new insights into the nature of Al promotion in Cu/ZnO-based catalysts.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Xin Zong,Yingmin Jin,Yumeng Li,Xuebai Zhang,Shiji Zhang,Haijiao Xie,Jinqiu Zhang,Yueping Xiong
Electrochemical CO 2 reduction (ECR) is a promising approach to realize carbon neutral and energy sustainability , which is still impeded by the low selectivity and activity for application. Defect engineering of electrocatalysts , especially oxygen vacancy introduction into metal oxide materials has been proved to be an effective strategy to satisfy thermodynamic condition and improve kinetics for ECR. Herein, we synthesize oxygen vacancy-enriched ZnO nanoparticle catalysts for efficient ECR through electrospinning technique using particular precursor. Characterizations reveal that the utilization of Zn(CH 3 COO) 2 precursor contributes to the generation of oxygen vacancies in ZnO catalysts which enhances CO 2 adsorption and stabilizes the intermediate. In a flow cell configuration, a current density of 150 mA cm −2 and a CO Faradic efficiency > 80% can be obtained for ZnO nanoparticle catalysts (p-ZnO-800), which is meaningful for industry.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 9
·4048-4053
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IF 3.5
Lin Gao,Guoqiang Ding,Lei Zhu,Zhanqiu Yu,Hongju Li,Guoqiang Li,Yulei Zhu,Hongwei Xiang,Xiaodong Wen,Yong Yang,Yongwang Li
The dimethyl maleate hydrogenation activity of Cu, ZnO-X and physically mixed Cu+ZnO-X samples was systematically investigated to probe the essential role of ZnO in ester hydrogenation processes. Cu samples exhibited high CC bond hydrogenation ability with dimethyl succinate as the main product. Comparatively, ZnO was inactive in hydrogenation due to its weak ability to dissociate hydrogen while the CO group could be activated and adsorbed on the ZnO surface. Interestingly, physical mixing with ZnO significantly improved the CO hydrogenation activity of Cu samples. The H2-TPD results reveal the origin of “Cu–ZnO synergy”: hydrogen atoms formed on the copper surface can spill over to the ZnO surface and react with the adsorbed CO group.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Tianqinji Qi,Weizuo Li,Hong Li,Ke Ji,Shaoyun Chen,Yongchun Zhang
Revealing the origin of the enhanced performance on yttria (Y 2 O 3 ) promoted Cu/ZnO based catalyst for methanol synthesis via CO 2 hydrogenation is still challenging. To shed light upon the promotion effect of Y 2 O 3 modifier on binary Cu/ZnO catalyst for CO 2 hydrogenation reaction, a ternary Cu/ZnO/Y 2 O 3 catalyst was synthesized via a citric acid coordination-assisted strategy. The developed Cu/ZnO/Y 2 O 3 catalyst exhibited a remarkably higher Weight-time yeild of methanol (236.8 g MeOH g cat −1 ∙ h − 1 ) and methanol selectivity (81.1%) in comparison to Cu/ZnO catalyst (159.6 g MeOH g cat −1 ∙ h − 1 and 73.9%, respectively). Various characterizations results have uncovered the enhanced catalytic activity of Cu/ZnO/Y 2 O 3 catalyst for methanol synthesis was associated with small size and highly dispersed Cu species and abundant surface adsorption sites as well as more Cu-ZnO interfaces with strong interaction. Moreover, the Cu/ZnO/Y 2 O 3 catalyst displayed a superior weight-time yield of methanol with a time-on-stream of 100 h in comparison with classic Cu/ZnO catalyst. We anticipate that this basic design strategy will provide a novel alternative to expand opportunities to explore scalable, cost-effective catalysts for industrial methanol synthesis.
研究领域:
化学工程
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催化科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Yihua Yue,Zhongliang Huang,Dongren Cai,Shafqat Ullah,Abdul-Rauf Ibrahim,Xin Yang,Jiale Huang,Guowu Zhan
Controlled fabrication of spatial positions of different active sites on catalyst structures is critical to exploring the reaction mechanisms for CO 2 hydrogenation. Herein, two isomorphous zeolitic imidazolate frameworks (ZIF-67 and ZIF-8) were used as sacrificial templates to synthesize multi-layered Co 3 O 4 /ZnO catalysts with tunable core-shell structures and well-controlled spatial positions. The multi-layered catalysts were then evaluated for the catalytic performance for CO 2 hydrogenation. A series of characterization techniques were applied to investigate the morphology and structure of the Co 3 O 4 /ZnO composites with different spatial locations. Due to the unique multi-layered structure, the distinct interfacial structures, and the synergistic effects, the resultant core-shell structured Co 3 O 4 /ZnO nanocatalysts exhibited significantly enhanced activity as compared to their monometallic counterparts (pure Co 3 O 4 and ZnO). In addition, the ZnO@Co 3 O 4 with Co 3 O 4 as shell showed significantly higher CO 2 conversion (25%) than that of Co 3 O 4 @ZnO with ZnO as shell (0.82%). Furthermore, in-situ Diffuse Reflection Fourier Transform Infrared Spectroscopy (DRIFTS) analysis suggested that formate (HCOO*) and methoxy (CH 3 O*) species were the crucial intermediates in the CO 2 hydrogenation over the Co 3 O 4 /ZnO composite nanocatalysts. However, pure ZnO could not activate the CO 2 ; consequently, the use of the Co 3 O 4 /ZnO nanocatalysts derived from multiple-layered ZIFs structures provides new insights into improving the catalytic efficiency of CO 2 hydrogenation.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Weifeng Tu,Chao Sun,Zhengzhou Zhang,Wenqi Liu,Haripal Singh Malhi,Wei Ma,Minghui Zhu,Yi-Fan Han
This work unravels the chemical and structural properties of Fe 5 C 2 -ZnO catalysts decorated with sodium (Na) during CO 2 hydrogenation to linear α-olefins, determined by rate assessments and series of in-situ characterizations. Reaction network remains as a combination of reverse water-gas-shift (RWGS) and CO hydrogenation, but their relative contributions vary. The RWGS reaction is chemically equilibrated, thus CO 2 conversion is determined solely by the thermodynamic constraint. However, Na addition alleviates the formation rates of paraffins from the subsequent CO hydrogenation and reactions of olefins with hydrogen. Na additive does not alter the structures of Fe 5 C 2 -ZnO, but improves largely the stability of Fe 5 C 2 by preventing the phase oxidation during the reaction. Na modifies the surface properties of catalyst, thus facilitates reaction of CO* and H* and the C C bond formation. The dual role of Na leads more effective olefins turnovers and provides new insights to the design of novel catalysts for CO 2 utilization.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）