Article
Energy & Fuels
Li Wang, Baojun Wang, Maohong Fan, Lixia Ling, Riguang Zhang
Summary: Engineering the surface structure of catalysts is an effective approach to modulate catalytic performance. This study designs a series of Pt-M (M = Au, Ag, and Cu) catalysts with different surface structures and reveals that adjusting the surface structure can effectively alter catalytic performance, which strongly depends on the ensemble size of active site and electronic properties. Among the considered Pt-M catalysts, PtCu3 IMC is found to be the most suitable catalyst with excellent C2H4 selectivity, higher activity, and good stability under the optimized experimental conditions of 520 K and a pH2:pC2H2 ratio of 10:1.
Article
Energy & Fuels
Yueyue Wu, Baojun Wang, Maohong Fan, Lixia Ling, Riguang Zhang
Summary: In this study, the role of S coverage in adjusting the active site spatial scale of Pd catalysts was investigated for regulating the catalytic performance of C2H2 selective hydrogenation. It was found that the catalytic performance strongly depends on the Pd active site spatial scale, which is influenced by the coverage of surface S species. The S/Pd-2 x 2 catalyst with a S coverage of 1/4 ML and a Pd active site spatial scale of 2.691 Å showed the best C2H4 activity and selectivity, as well as excellent catalyst stability.
Article
Engineering, Chemical
Yong-Zhi Li, Rajamani Krishna, Fan Xu, Wan-Fang Zhang, Yanwei Sui, Lei Hou, Yao-Yu Wang, Zhonghua Zhu
Summary: In this study, a novel microporous Cd-MOF material was constructed with a high C2H2 adsorption capacity, which can efficiently separate C2H2 from gas mixtures. The experimental results and molecular simulation demonstrated the importance of this material in acetylene separation.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Engineering, Environmental
Chenyang Lu, Shihong Zhou, Wenyu Zhou, Cailong Zhou, Qun Li, Aonan Zeng, Anjie Wang, Luxi Tan, Lichun Dong
Summary: A highly selective acetylene selective hydrogenation catalyst (Cu15Pd@C) was successfully prepared, which improves ethylene selectivity while maintaining high activity. The carbon layer promotes the formation of smaller nanoparticles and effectively inhibits the production of green oil associated with acetylene coupling. The same approach was applied to fabricate a series of carbon-confined Cu and Ag-based bimetal catalysts, demonstrating the universality and potential applications of the carbon layer in selective hydrogenation.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Chemical
Yamin Qi, Xiuxiu Shao, Baojun Wang, Debao Li, Lixia Ling, Riguang Zhang
Summary: The study investigates the influence of shell Pd ensemble form on the catalytic performance of core-shell Pd@M catalysts in C2H2 semi-hydrogenation. It is found that the C2H4 selectivity and activity are closely related to the shell Pd ensemble form, with different forms having different effects. Moderately located d-band center plays a positive role in reaction performance, suggesting that controlling the ensemble form of shell Pd may be a method to adjust catalytic performance.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Nanoscience & Nanotechnology
Yueyue Wu, Wantong Zhao, Yuan Wang, Baojun Wang, Maohong Fan, Riguang Zhang
Summary: Research shows that the type and coverage of subsurface heteroatoms have significant effects on the catalytic performance of C2H2 semihydrogenation. Pd-B0.5 and Pd-C0.5 catalysts exhibit the best performance, improving selectivity and activity while effectively suppressing by-products. Subsurface heteroatoms tune catalytic performance by altering the electronic and geometric structures of the Pd surface.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Chemical
Ying Wang, Wenjuan Zheng, Baojun Wang, Lixia Ling, Riguang Zhang
Summary: This study investigated the catalytic performance of PdM (M = Cu, Ag, Au) IMCs with different Pd/M ratios in the C2H2 semi-hydrogenation reaction using DFT calculations. The results showed that Pd1Cu3, Pd1Ag1 and Pd1Au1 IMCs catalysts exhibited better activity and selectivity, with PdCu3 as the most suitable catalyst due to the presence of surface isolated Pd atoms as active sites. This research provides valuable insights for the design of IMCs-containing Pd catalysts in C2H2 semi-hydrogenation, with broad implications for the development of such catalysts.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Nanoscience & Nanotechnology
Yuan Wang, Yueyue Wu, Xinyi Guo, Baojun Wang, Maohong Fan, Riguang Zhang
Summary: This study investigates the impact of heteroatom doping on the catalytic performance of transition metal surfaces through calculations and simulations. The results show that the type of doped heteroatom and the surface structure of Cu play crucial roles in C2H2 selective hydrogenation. High-coordination Cu(111) surfaces exhibit improved catalytic performance after heteroatom doping.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Chemical
Yamin Qi, Baojun Wang, Maohong Fan, Debao Li, Riguang Zhang
Summary: DFT calculations show that PdCu with surface Pd coordination number of 8 exhibits the best selectivity and activity towards C2H4 formation in the semi-hydrogenation process, while effectively inhibiting green oil formation. This study provides valuable insights for designing other metal alloyed single-atom Pd catalysts by controlling the coordination number and environment of single-atom Pd.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Jiaqi Liu, Kang Zhou, Saif Ullah, Jiafeng Miao, Hao Wang, Timo Thonhauser, Jing Li
Summary: A systematic study is conducted on the engineering of pore dimensions and pore functionality of fcu-type Y-based metal-organic frameworks (Y-MOFs) using different linear dicarboxylate linkers. The research demonstrates how slight changes in pore size and pore surface chemistry can affect the adsorption preference of C2H6, C2H4, and C2H2 by the MOFs, establishing clear relationships between pore size/pore surface polarity and C-2 adsorption selectivities. A specific compound, HIAM-326, shows remarkable preferential adsorption of C2H6 and C2H2 over C2H4, enabling the one-step purification of C2H4 from C2H6/C2H4/C2H2 ternary mixtures to obtain high purity C2H4 (99.9%+).
Article
Engineering, Chemical
Arun Pal, Shyam Chand Pal, Hui Cui, Rui-Biao Lin, Dipankar Singha, Malay Kumar Rana, Banglin Chen, Madhab C. Das
Summary: A three-dimensional metal-organic framework (IITKGP-30) with narrow pore channels was developed for efficient separation of C2H2 from C2H4, exhibiting excellent separation selectivity and stability.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Maxim Zabilskiy, Vitaly L. Sushkevich, Mark A. Newton, Frank Krumeich, Maarten Nachtegaal, Jeroen A. van Bokhoven
Summary: Catalysts based on Pd-Zn alloy typically produce CO instead of methanol, indicating that the presence of a ZnO phase in contact with the Pd-Zn phase is crucial for efficient methanol production. Mechanistic studies showed that the Pd-Zn phase alone does not provide the necessary active sites for methanol production through direct hydrogenation of carbon dioxide.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Environmental Sciences
Jingya Sun, Kun Liu, Pedro J. J. Alvarez, Heyun Fu, Shourong Zheng, Daqiang Yin, Xiaolei Qu
Summary: In this study, TiO2-supported Pd catalysts were used to selectively hydrogenate the C--C bonds in the Adda moiety of MC-LR, achieving rapid detoxification in water. Catalytic hydrogenation significantly decreased the toxicity of MC-LR by 90.8% within 30 minutes, demonstrating effective detoxification. Surface adsorption and cationic Pd played crucial roles in the reaction kinetics.
Article
Engineering, Chemical
Yadan Du, Yang Chen, Yong Wang, Chaohui He, Jiangfeng Yang, Libo Li, Jinping Li
Summary: A metal-organic framework has been developed for efficient adsorptive separation of acetylene and ethylene mixtures, showing outstanding separation performance and selectivity.
SEPARATION AND PURIFICATION TECHNOLOGY
(2021)
Article
Engineering, Chemical
Shidong Wang, Yaxi Wang, Xinru Wu, Cejun Hu, Hongwei Zhang, Qinyang Cui, Xiaojun Bao, Pei Yuan
Summary: Pore diffusion plays a significant role in the heterogeneous hydrogenation of unsaturated polymers. The influence of pore size on the hydrogenation activity of nitrile butadiene rubber (NBR) was investigated using a series of Pd/SiO2 catalysts with graded pore sizes. It was found that when the catalyst pore size was 7 times larger than the diameter of NBR chains, the internal mass transfer limitation could be eliminated, resulting in excellent catalytic activity (96.7%) and selectivity (100%) towards C=C. This study highlights the importance of pore size in regulating pore diffusion limitation and the accessibility of internal active sites in macromolecular hydrogenation catalyst design.
CHEMICAL ENGINEERING SCIENCE
(2023)
Review
Chemistry, Multidisciplinary
Runping Ye, Yuan-Yuan Huang, Chong-Chong Chen, Yuan-Gen Yao, Maohong Fan, Zhangfeng Zhou
Summary: This article reviews various approaches to synthesize ethylene glycol (EG) from CO2 and its derivatives under mild conditions, including thermocatalysis, photocatalysis, and electrocatalysis. The coal-to-ethylene glycol technology, a mature thermal catalytic method, still faces challenges in industrialization. The recent progress in the development of coal-to-ethylene glycol technology is discussed, with a focus on achieving EG synthesis under mild conditions through strategies such as doping promoters, support modification, and catalyst design. The emerging technological progress of photocatalytic and electrocatalytic EG synthesis under ambient conditions is also introduced, highlighting the need to address issues for large-scale production. Future development issues and prospects for ambient EG synthesis using different catalytic routes are proposed.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Lulu Ping, Yuan Zhang, Baojun Wang, Maohong Fan, Lixia Ling, Riguang Zhang
Summary: Based on the advantages of ethane oxidative dehydrogenation and the challenge of low ethylene selectivity, chemical looping oxidative dehydrogenation (CL-ODH) over the IrO2 catalyst was studied. The study revealed that both S-IrO2 and R-IrO2 states exist for the IrO2 catalyst in the dehydrogenation and regeneration processes, and the optimal reaction conditions were determined. This research expands the understanding of ethane CL-ODH over metal oxide catalysts and provides valuable information for process optimization and catalyst development.
Article
Nanoscience & Nanotechnology
Yuan Zhang, Baojun Wang, Maohong Fan, Lixia Ling, Riguang Zhang
Summary: In this study, a strategy to improve the catalytic performance of Pt-Sn alloy catalysts in ethane dehydrogenation (EDH) is proposed by engineering the shell surface structure and thickness. Density functional theory (DFT) calculations and kinetic Monte Carlo (kMC) simulations are used to understand the influences of catalyst surface structure, temperature, and reactant partial pressures. The results demonstrate that Pt@Pt3Sn catalysts generally have higher C2H4(g) activity and lower selectivity compared to Pt3Sn@Pt catalysts, due to their unique surface geometrical and electronic properties.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Lulu Chai, Jinlu Song, Yanzhi Sun, Xiaoguang Liu, Xifei Li, Maohong Fan, Junqing Pan, Xueliang Sun
Summary: This study proposes a smart dual-oxygen electrode for high-specific-energy batteries, which addresses the issues of energy efficiency decay, wide charge-discharge gap, and catalyst peeling. The electrode consists of a switch control module, OER and ORR catalysis layers, and an ion conductive | electronic insulating membrane. The electrode shows an ultralow energy efficiency decay rate and enables a high energy efficiency in zinc-air batteries.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Wantong Zhao, Xuebai Lan, Baojun Wang, Maohong Fan, Riguang Zhang
Summary: In this study, the inverse Mo6C4/Cu catalyst is modeled and predicted to promote C2 oxygenates formation in syngas transformation. The results show that the inverse Mo6C4/Cu catalyst greatly improves catalytic performance and facilitates C2 oxygenate production compared to previous catalysts. This is attributed to the synergistic effect between Mo6C4 cluster with Cu catalyst, which easily activates CO to produce CH2 monomer and facilitates CO insertion into CH2 to CH2CO.
APPLIED SURFACE SCIENCE
(2023)
Article
Energy & Fuels
Kunpeng Li, Hui Hu, Maohong Fan, Mi Zhang, Zhongming Chen, Ruibin Lv, Hao Huang
Summary: An advanced oxidation process (AOPs) using Fe(II) activated peracetic acid (PAA) was investigated for the simultaneous removal of SO2 and NO from flue gas. The maximum removal efficiencies obtained were 92.3% for NO and 99.5% for SO2 under optimal conditions. Reactive oxidizing species and organic radicals were generated in the Fe(II)/PAA system, with organic radicals confirmed to be the major factors affecting NO oxidation. The main products of SO2 and NO removal were identified as SO42- and NO3-.
Review
Chemistry, Multidisciplinary
Tongtong Wang, Zhe Chen, Weibo Gong, Fei Xu, Xin Song, Xin He, Maohong Fan
Summary: Carbon nanofibers (CNFs) have diverse applications in sensor manufacturing, electrochemical catalysis, and energy storage. Electrospinning is a powerful commercial large-scale production technique for CNFs due to its simplicity and efficiency. This paper discusses the working theory of manufacturing electrospun CNFs, current efforts in upgrading CNF properties, and the corresponding applications. Future development of CNFs is also discussed.
Article
Chemistry, Physical
Yueyue Wu, Xinyi Guo, Xiufeng Shi, Baojun Wang, Maohong Fan, Riguang Zhang
Summary: This study investigates the catalytic performance of a series of S-modified PdM IMCs with different M types (Cu, Ag and Au) and ratios (1: 1, 3: 1 and 1: 3) in C2H2 semi-hydrogenation using DFT calculations and microkinetic modeling. The results show that the catalytic performance strongly depends on the space region of metal active site and the electronic properties induced by S atoms and the M type and ratio. Only S/Pd1Ag1 and S/Pd1Au1 exhibit higher H2 dissociation activity, C2H4 selectivity and production activity, and can effectively inhibit the formation of green oil.
APPLIED SURFACE SCIENCE
(2023)
Article
Energy & Fuels
Weixiang Zhang, Lina Zhang, Sijia Pei, Jiarui Wang, Dawei Liu, Xiaoxun Ma, Maohong Fan, Long Xu
Summary: One of the most significant topics in chemical looping reforming technology is the design and preparation of appropriate oxygen carriers with high reactivity and excellent stability. This study focuses on the chemical looping reforming of methane using cobalt-doped Ce-based oxygen carriers synthesized via the solution combustion method with the assistance of coconut shell. The introduction of cobalt decreases the crystallite size, increases oxygen vacancy concentration and lattice oxygen mobility, and the addition of coconut shell further enhances these positive changes and the interaction between Ce and Co.
Editorial Material
Multidisciplinary Sciences
Jie Ding, Runping Ye, Yanghe Fu, Yiming He, Ye Wu, Yulong Zhang, Qin Zhong, Harold H. Kung, Maohong Fan
Summary: Urea, a crucial nitrogen fertilizer, plays a vital role in meeting global food demand. However, its current production method is energy-intensive and environmentally unfriendly. In this commentary article, the authors propose strategies to address and overcome these challenges.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Zhao Sun, Shufan Yu, Sam Toan, Rufat Abiev, Maohong Fan, Zhiqiang Sun
Summary: In this study, CuCr2O4-based catalytic oxygen carriers were designed for low-temperature methanol reforming. The activation of methanol at relatively low temperatures was achieved through the reinforcement of the Cu-O-Cr structure and the induction of highly reactive lattice oxygen. The hydrogen production rate was significantly increased by 53.2% with the application of CuCr2O4-based catalytic oxygen carriers. Furthermore, the Cu-O-Cr structure demonstrated satisfactory cyclic stability.
Article
Chemistry, Physical
Lulu Ping, Yuan Zhang, Baojun Wang, Maohong Fan, Lixia Ling, Riguang Zhang
Summary: Based on favorable thermodynamics and coking resistance, chemical looping oxidative dehydrogenation (CL-ODH) of ethane over IrO2 catalyst was studied. Two extreme states of the IrO2 surface structure, S-IrO2 and R-IrO2, were considered. It was found that the mechanisms of ethane dehydrogenation over S-IrO2 and R-IrO2 catalysts were different. The present study contributes to the understanding of ethane CL-ODH over metal oxide catalysts and provides valuable insights for process optimization and catalyst development.
Article
Chemistry, Multidisciplinary
Runping Ye, Lixuan Ma, Xiaoling Hong, Tomas Ramirez Reina, Wenhao Luo, Liqun Kang, Gang Feng, Rongbin Zhang, Maohong Fan, Riguang Zhang, Jian Liu
Summary: This study presents a strategy to enhance the low-temperature CO2 activation through regulating the local electron density of active sites. An optimized Ni/ZrO2 catalyst exhibits excellent performance for CO2 methanation, with high CO2 conversion, CH4 selectivity, and stability, making it one of the best Ni-based catalysts for CO2 methanation to date.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Xuebai Lan, Mifeng Xue, Baojun Wang, Maohong Fan, Riguang Zhang
Summary: This study investigates the performance of diatomic metal catalysts in the semi-hydrogenation of C2H2 by constructing different types of DACs and tuning their coordination environments. The results show that CoCu@N6V4-11, CoPd@N6V4-11, CoNi@N6V4-11, and CoPt@N6V4-11 DACs exhibit superior C2H4 selectivity, formation activity, and stability. Introducing a second metal can significantly improve C2H4 selectivity while maintaining high C2H4 formation activity.
APPLIED SURFACE SCIENCE
(2023)