Article
Chemistry, Applied
Hangjie Li, Liang Wang, Feng-Shou Xiao
Summary: By introducing silica promoter, the Cu/ZnO/Al2O3 catalyst has achieved significantly improved methanol selectivity and catalyst durability.
Article
Chemistry, Physical
Jincheng Wu, Guoguo Liu, Qin Liu, Yajing Zhang, Fu Ding, Kangjun Wang
Summary: We have developed a highly efficient and cost-effective Cu-SiO2 catalyst using the ammonia-evaporation method. This catalyst demonstrated superior performance with a methyl formate conversion of 94.2% and a methanol selectivity of 99.9% in the liquid product. Compared to the commonly used Cu-Cr catalyst, the Cu-SiO2 catalyst exhibited higher conversion and yield under the same reaction conditions, thanks to the presence of Si-OH groups which enhanced the hydrogen spillover effect and prevented sintering. This study provides a strategy for the rational design of efficient catalysts for industrial applications.
Article
Energy & Fuels
Xingzi Wang, Hai Zhang, Huang Qin, Kunming Wu, Kai Wang, Junfang Ma, Weidong Fan
Summary: This work investigates the hydrogenation of CO2 to methanol over Cu/ZnO-based catalyst by focusing on the mechanism and interface effects. Atomic doping of Cu/ZnO-X(Al,Mg,Ga,Pt,Pd,Au) catalyst was simulated to study the enhancing effect of metal promoters. Density functional theory (DFT) calculation was conducted to analyze the adsorption, thermodynamics, and kinetics of CO2 methanolization. The simulation results provide guidance for the design of high-efficiency catalysis for CO2 hydrogenation and are consistent with previous experimental results.
Article
Chemistry, Physical
Xiaojing Cui, Yequn Liu, Yangang Mei, Jiamei Li, He Zhang, Shanhui Zhu, Yulan Niu, Tiansheng Deng
Summary: A surface silylation method is found to efficiently suppress the reverse water-gas-shift reaction on a commercial Cu/ZnO/Al2O3 catalyst, leading to improved methanol selectivity and yield.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Engineering, Environmental
Jiyu Sun, Fangyuan Liu, Usman Salahuddin, Mudi Wu, Chunxiang Zhu, Xingxu Lu, Bo Zhang, Binchao Zhao, Zhiqiang Xie, Yunjiang Ding, Dongsheng Li, Chang-Yong Nam, Feng-Yuan Zhang, Pu-Xian Gao
Summary: By tuning the experimental processing parameters, highly improved ZnO nanoarray supported Cu-ZnO-Al2O3 catalysts have been successfully demonstrated for methanol production under low-temperature and low-pressure conditions, with desirable yield and selectivity.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Itzhak I. Maor, Svetlana Heyte, Oren Elishav, Meirav Mann-Lahav, Joelle Thuriot-Roukos, Sebastien Paul, Gideon S. Grader
Summary: A new architecture of Cu- and Cu/Zn-based catalysts supported on electrospun alumina nanofibers was synthesized for the synthesis of methanol and DME from CO2 and green hydrogen. The hierarchical fibrous structure of the catalyst played a crucial role in the reaction activity and selectivity. The Cu or Cu/ZnO formed a unique nanosheet structure, providing a large surface area for the reaction. The catalysts containing 7% wt. Cu/Zn with a weight ratio of 2.3 Zn to Cu achieved maximal production of methanol and DME.
Article
Chemistry, Applied
Youwei Yang, Dawei Yao, Mengjiao Zhang, Antai Li, Yueqi Gao, Busha Assaba Fayisa, Mei-Yan Wang, Shouying Huang, Yue Wang, Xinbin Ma
Summary: A series of Mo-doped Cu/SiO2 catalysts were prepared and used for the hydrogenation of ethylene carbonate (EC), with the 0.5 wt% Mo-doped catalyst exhibiting the highest catalytic performance. The addition of Mo can enhance copper dispersion and prevent aggregation, leading to improved activation of EC. The insights gained from this study may help in designing more efficient copper-based catalysts for the hydrogenation of carbon-oxygen bonds.
Article
Chemistry, Physical
Yuxin Wang, Yayu Wei, Yanhong Li, Xiaofang Chen, Juergen Caro, Aisheng Huang
Summary: The formation of methanol from CO2 hydrogenation is a topic of great interest in terms of carbon resource utilization. However, this transformation is challenging due to thermodynamic equilibrium restriction and water-caused catalyst deactivation. Therefore, the development of highly active, selective, and stable catalysts for CO2 hydrogenation to methanol is highly desired. In this study, a novel tandem catalyst composed of CZAZ and Cu-MOR is proposed, which achieves highly selective conversion of CO2 to methanol. The by-product methane is continuously transformed to methanol through reaction with water, enhancing CO2 conversion and methanol selectivity. High CO2 conversion (40.7%) and methanol selectivity (97.6%) are achieved under mild reaction conditions, outperforming state-of-the-art CO2 hydrogenation catalysts. Furthermore, the water-caused deactivation of the catalyst is suppressed, validating a high stability of the CZAZ/Cu-MOR tandem catalyst.
Article
Engineering, Environmental
Fei Chen, Jiaming Liang, Fan Wang, Xiaoyu Guo, Weizhe Gao, Yasuharu Kugue, Yingluo He, Guohui Yang, Prasert Reubroycharoen, Tharapong Vitidsant, Noritatsu Tsubaki
Summary: Surface modification is an efficient strategy to enhance the activity and stability of traditional Cu/ZnO catalyst in methanol synthesis. This study focuses on the influence of boron oxide (B2O3) modification on Cu/ZnO catalyst, revealing a balance between the promotional effect of B2O3 and the negative influence caused by excessive B2O3. The CZB-R-0.05 catalyst exhibits significantly improved methanol yield and stability, as well as reduced activation energy for low-temperature methanol synthesis.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Tianqinji Qi, Weizuo Li, Hong Li, Ke Ji, Shaoyun Chen, Yongchun Zhang
Summary: The research findings suggest that the addition of yttria (Y2O3) can enhance the performance of the Cu/ZnO catalyst for CO2 hydrogenation to methanol. The newly synthesized Cu/ZnO/Y2O3 catalyst showed higher methanol yield and selectivity due to small, well-dispersed Cu species, abundant surface adsorption sites, and more Cu-ZnO interfaces. This basic design strategy offers a promising approach for developing scalable and cost-effective catalysts for industrial methanol synthesis.
MOLECULAR CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Jian Wang, Xiuli Qu, Xavier Djitcheu, Qingrun Meng, Zenan Ni, Huimin Liu, Qijian Zhang
Summary: The emergence of the double carbon era has raised significant concerns in CO2 utilization. CO2 conversion to methanol is considered a promising method, and the use of photo-assisted reactions has been found to improve its efficiency. A study on Cu-ZnO and Cu-ZnO-ZrO2 catalysts showed that the latter exhibited higher methanol selectivity and further improvement with the photo-assisted reaction. This superior performance was attributed to the increased oxygen vacancies on the ZnO surface, which enhanced the catalyst's ability to reduce CO2 to methanol under light irradiation.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Physical
Andraz Mavric, Gregor Zerjav, Blaz Belec, Matevz Roskaric, Matjaz Finsgar, Albin Pintar, Matjaz Valant
Summary: The performance of Cu/ZnO catalyst system with AlMg-oxide phase in CO2 hydrogenation to methanol was studied. The catalyst was prepared by thermal treatment of hydrotalcite phase with mixed metal cations. During the hydrogenation reaction, CuO in the presence of ZnO and disordered AlMg-oxide phase was easily reduced to Cu. The catalyst showed stable catalytic activity at relatively low Cu metal content (around 14 at.%) with constant space-time yield for methanol and high methanol selectivity (>85%).
Article
Engineering, Environmental
Zheng Li, Yihui Li, Xuepeng Wang, Yuan Tan, WenShao Yang, Hejun Zhu, Xingkun Chen, Wei Lu, Yunjie Ding
Summary: The hydrogenation of dimethyl oxalate to produce ethanol is a research topic of great interest due to its environmentally friendly nature. However, the yield of ethanol using Cu-based catalysts remains a challenge. In this study, a molybdenum-doped Cu catalyst was synthesized and demonstrated to be a robust catalyst with a high ethanol yield. The addition of Mo increased the amount of surface Cu+ species and enhanced the surface acidity, resulting in a high ethanol selectivity.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Energy & Fuels
Hao Chen, Haishuai Cui, Yang Lv, Pingle Liu, Fang Hao, Wei Xiong, He'an Luo
Summary: Cu/ZnO/ZrO2 catalysts with different ZnO morphologies were prepared and used for CO2 hydrogenation to methanol. The catalyst with flower-like ZnO morphology showed the highest catalytic performance and possess the most oxygen vacancies. The experimental results and DFT calculations suggest that oxygen vacancies play a crucial role in promoting the reaction and reducing the energy barriers.
Article
Chemistry, Physical
Xiao Chang, Xiaohui Zi, Jing Li, Fengdong Liu, Xiaoyu Han, Jiyi Chen, Ziwen Hao, Heng Zhang, Zhenmei Zhang, Pengju Gao, Maoshuai Li, Jing Lv, Xinbin Ma
Summary: The study examines the effect of ZnO and ZrO2 composition on the structure and surface properties of Cu/ZnO/ZrO2 catalyst, revealing a synergistic interaction between Cu and oxides (ZnO and ZrO2) that enhances methanol synthesis. The optimized Cu/ZnO/ZrO2 catalyst exhibits higher methanol yield compared to the traditional Cu/ZnO/Al2O3 catalyst.
Article
Chemistry, Physical
Ting Wang, Chengguang Yang, Peng Gao, Shiju Zhou, Shenggang Li, Hui Wang, Yuhan Sun
Summary: In this study, a series of bifunctional catalysts composed of highly active ZnZrOx oxides and nanocrystal HZSM-5 zeolites were used to achieve direct CO2 hydrogenation into aromatics with high selectivity. The extension of the b-axis length of HZSM-5 was found to increase the selectivity of para-xylene (PX) while shortening the length favored the formation of tetramethylbenzene (TeMB), with maximum selectivities reaching 28.9% and 74.1%, respectively.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Engineering, Chemical
Ziwei Wang, Hao Wang, Chengguang Yang, Sheng Wang, Peng Gao, Yuhan Sun
Summary: Bifunctional catalysts using hierarchical ZSM-5 zeolite as a support have attracted attention for their ability to produce middle distillate hydrocarbons in Fischer-Tropsch synthesis. The hierarchical ZSM-5 zeolites with varying acidities and mesopore volumes are synthesized by treating zeolites with TPAOH solution, leading to enhanced CO conversion and production of heavier hydrocarbons with increased cobalt loading.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Bin Qin, Zhimin Zhou, Shenggang Li, Peng Gao
Summary: Utilizing density functional theory calculations, this study thoroughly investigated the reaction mechanisms and catalytic activities of methanol and CO formations from CO2 hydrogenation at different surface oxygen vacancy sites on stable cubic In2O3 surfaces, establishing a structure-performance relationship. Results showed that the stability of reaction intermediates and formation energy of the Ov sites can determine the rate-determining step for CH3OH formation, while linear regression analysis was used to establish relationships between activation barriers and reaction energies for different steps. Moreover, the study suggested that Ov sites with different coordinations favor different reaction pathways for methanol and CO formation.
JOURNAL OF CO2 UTILIZATION
(2021)
Article
Chemistry, Physical
Xiaosu Dong, Shuxin Ma, Peng Gao
Summary: CO2 conversion to CH3OH is crucial for energy and environmental development. The preparation of high-performance Cu-based catalysts with high Cu dispersion remains challenging. This study presents a liquid reduction strategy without calcination to improve catalytic reactivity. Different preparation methods and calcination procedures significantly affect the performance of Cu-based catalysts. Uncalcined catalysts exhibit better performance, and liquid reduction method has potential for the design of highly dispersed metal nanoparticles catalysts.
Review
Chemistry, Multidisciplinary
Peng Gao, Liangshu Zhong, Buxing Han, Mingyuan He, Yuhan Sun
Summary: The concept of green carbon science aims to achieve carbon neutrality, which has gained global recognition and attention. The transition from fundamental research to practical applications in addressing the urgent need for carbon neutralization must be accelerated. This Review summarizes recent technological developments in the field of green carbon science, focusing on pilot tests, industrial demonstrations, and commercial applications beyond the laboratory stage.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Haiyan Yang, Yaru Dang, Xu Cui, Xianni Bu, Jiong Li, Shenggang Li, Yuhan Sun, Peng Gao
Summary: This study fabricated zinc- and sodium-modulated iron catalysts, which exhibited the best activity and stability. Copper was found to decrease the energy barrier of the rate-determining step for olefin hydrogenation and result in a lower olefin-to-paraffin ratio. The ZnO/Fe5C2 interface facilitated olefin desorption and inhibited the undesirable secondary reaction of olefins, enabling a high selectivity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Yuchen Wang, Liang Zhu, Yang Liu, Evgeny I. Vovk, Junyu Lang, Zixuan Zhou, Peng Gao, Shenggang Li, Yong Yang
Summary: The In2O3 catalyst shows high activity for CO2 hydrogenation to methanol. In this study, in situ IR and XPS techniques are used to investigate the O1s binding energies of adsorbates induced by CO2 and H2O treatments. Computational simulations are also performed to correlate the assignments with surface structures. The results provide valuable information for understanding the surface structure of the In2O3 catalyst and its behavior during methanol synthesis.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Junyu Lang, Yulu Cai, Zhehao Qiu, Peng Gao, Yong Yang
Summary: Indium oxide (In2O3) has shown great potential as a catalyst for the selective hydrogenation of CO2 to methanol, a green energy fuel. In this study, the H-2/D-2 isotope effects on the catalytic methanol synthesis were investigated using online MS measurements. The results revealed a higher activation energy for D-2/CO2 compared to H-2/CO2 inputs. The study also showed that the active surface is highly reduced by hydrogen and has a high efficiency in converting surface hydrogen to methanol.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Haojie Liang, Bin Zhang, Peng Gao, Xiaohu Yu, Xingchen Liu, Xinchun Yang, Huibin Wu, Liming Zhai, Shichao Zhao, Guofu Wang, Alexander P. van Bavel, Yong Qin
Summary: In this study, superstable Co single atom catalysts were synthesized using atomic layer deposition method, showing high CO selectivity and stability, and a reaction mechanism was proposed.
Article
Chemistry, Physical
Hao Wang, Peng Gao, Shenggang Li, Ting Wang, Chengguang Yang, Jiong Li, Tiejun Lin, Liangshu Zhong, Yuhan Sun
Summary: We fabricated a high-performance bifunctional catalyst for the direct conversion of syngas to aromatics. The catalyst, comprising Co2C nanoprisms and HZSM-5@silicalite-1 zeolites, showed high activity and stability, achieving a high CO conversion and selectivity towards aromatics, leading to a high space-time yield of PX.
Article
Chemistry, Multidisciplinary
Zhou Zixuan, Yang Haiyan, Sun Yuhan, Gao Peng
Summary: The utilization of fossil fuels has brought prosperity to human society but has also led to negative impacts such as increased carbon dioxide emissions and global temperature rise. The depletion of fossil fuels necessitates the search for alternative carbon sources for sustainable development. Utilizing green hydrogen obtained from renewable sources, the hydrogenation of CO2 to methanol offers an efficient and clean solution for both excess CO2 utilization and renewable methanol production.
CHEMICAL JOURNAL OF CHINESE UNIVERSITIES-CHINESE
(2022)
Article
Chemistry, Applied
Zixuan Zhou, Peng Gao
Summary: This study summarizes the progress in the rational design and construction of efficient catalysts for CO2 hydrogenation to produce chemicals and liquid fuels. The structure-performance relationship, nature of the active sites, and reaction mechanisms of these catalysts are explored using computational and experimental evidence. The results of this study will promote further fundamental research and industrial applications in the field.
CHINESE JOURNAL OF CATALYSIS
(2022)
Article
Multidisciplinary Sciences
Lei Zhang, Yaru Dang, Xiaohong Zhou, Peng Gao, Alexander Petrus van Bavel, Hao Wang, Shenggang Li, Lei Shi, Yong Yang, Evgeny Vovk, Yihao Gao, Yuhan Sun
Summary: A study on a Na-modified CoFe alloy catalyst demonstrated high selectivity in transforming CO2 into jet fuel, providing a promising technique for eco-friendly and carbon-neutral fuel production.
Article
Chemistry, Multidisciplinary
Hao Wang, Ziwei Wang, Sheng Wang, Chengguang Yang, Shenggang Li, Peng Gao, Yuhan Sun
Summary: A series of mesoporous ZSM-5 zeolite supported cobalt-based catalysts were prepared for syngas conversion, with cobalt crystal sizes ranging from 4.5-18.1 nm, enabling highly selective synthesis of various liquid fuels including gasoline, jet fuel, and diesel range hydrocarbons using different cobalt nanoparticle sizes.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Applied
Siyu Lu, Haiyan Yang, Zixuan Zhou, Liangshu Zhong, Shenggang Li, Peng Gao, Yuhan Sun
Summary: In this study, In2O3 with varying particle sizes and SAPO-34 were used as bifunctional catalysts for CO2 hydrogenation, revealing that decreasing the average In2O3 crystallite size can enhance the CO2 conversion and selectivity of lower olefins. However, In2O3 particles smaller than 19 nm are more prone to sintering.
CHINESE JOURNAL OF CATALYSIS
(2021)