Article
Chemistry, Multidisciplinary
Selina K. Kaiser, Adam H. Clark, Lucrezia Cartocci, Frank Krumeich, Javier Perez-Ramirez
Summary: A new synthesis method has been developed to prepare carbon-supported gold nanostructures in bimetallic catalysts, allowing for atomic-level gold dispersion to address the practical applicability of gold single-atom catalysts. Platinum plays a key role in promoting a chlorine-mediated dispersion mechanism, preventing sintering of gold agglomerates and maintaining the activity of Au(I)-Cl active sites.
Article
Chemistry, Physical
Yurui Fan, Haomiao Xu, Zhisong Liu, Songyuan Sun, Wenjun Huang, Zan Qu, Naiqiang Yan
Summary: This study demonstrates the synergistic effect of Cu(X) on the catalytic activity and selectivity of the acetylene hydrochlorination reaction. The findings provide guidance for designing efficient Ru-based catalysts and solutions for replacing mercury-contained catalysts in engineering applications.
Article
Chemistry, Physical
Tiantong Zhang, Bao Wang, Yao Nian, Menghui Liu, Yiming Jia, Jinli Zhang, You Han
Summary: In this study, the active sites on Cu-based catalysts for acetylene hydrochlorination were investigated. It was found that the indirect ligand-coordinated sites induced by excess copper chloride exhibited superior performance. Molecular dynamics simulation and density functional theory calculations revealed that excess copper chloride molecules spontaneously formed chain structures, leading to the formation of indirect ligand-coordinated sites and electron transfer along the copper chloride chain, which were crucial for the high catalytic activity. These findings provide fundamental insights into the origin of activity and the identification of active sites in Cu-ligand catalysts for acetylene hydrochlorination.
Article
Chemistry, Physical
Yang Yang, Chaoyue Zhao, Xianliang Qiao, Qingxin Guan, Wei Li
Summary: DFT calculations were used to predict the catalytic activities of metal single-atom catalysts with nitrogen coordination in acetylene hydrochlorination. The results showed that Ru-Nx SACs had the best catalytic performance. Ru-Nx SACs were fabricated by pyrolyzing MOFs with in-situ spatially confined metal precursors, and the N coordination environment was controlled by changing the pyrolysis temperature. Catalytic performance tests indicated that low N coordination number (Ru-N2, Ru-N3) showed excellent activity and stability. DFT calculations further revealed the preference of Ru-N2 and Ru-N3 for activating HCl and Ru-N4 for activating C2H2. These findings provide a reference for the design and control of metal active sites.
GREEN ENERGY & ENVIRONMENT
(2023)
Article
Chemistry, Physical
Bolin Wang, Yuxue Yue, Saisai Wang, Shujuan Shao, Zhi Chen, Xianhua Fang, Xiangxue Pang, Zhiyan Pan, Jia Zhao, Xiaonian Li
Summary: The study introduces an innovative strategy of coating an ionic liquid film on the surface of gold (Au) catalysts to construct an acetylene-deficient reaction phase, which enhances catalytic stability. Furthermore, kinetic and theoretical analysis demonstrate that this constructed reaction phase can inhibit the reduction of gold and generation of carbon deposition.
GREEN ENERGY & ENVIRONMENT
(2021)
Article
Chemistry, Physical
Yuliang Zhou, Yuan Wang, Lixia Ling, Baojun Wang, Riguang Zhang
Summary: The study reveals the impact of the metal M type and local coordination environment in N-doped graphene anchored RuM diatomic catalysts on C2H2 hydro-chlorination activity, identifying five catalyst types with excellent performance. By tuning the local coordination environment and types of the second metal M, high-performance and low-cost RuM diatomic catalysts can be rationally designed for industrial applications.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Jian Li, Haiyang Zhang, Haixia Liang, Linfeng Li, Jinli Zhang
Summary: In this study, Ru-L-x/AC catalysts were synthesized to address the issues of traditional Ru/AC catalyst and improve the activity and stability of acetylene hydrochlorination reaction. The newly developed catalyst showed significantly improved performance and has great potential for industrial applications.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Physical
Samuel Pattisson, Simon R. Dawson, Grazia Malta, Nicholas F. Dummer, Louise R. Smith, Anna Lazaridou, David J. Morgan, Simon J. Freakley, Simon A. Kondrat, Joost J. Smit, Peter Johnston, Graham J. Hutchings
Summary: The commercialization of gold for acetylene hydrochlorination is a significant achievement in the field. The development of second-generation gold catalysts aims to enhance their activity and stability. This study demonstrates that the surface oxygen content of carbon-based gold catalysts affects their activity. By modifying the Hummers chemical oxidation method before gold deposition, the oxygen content of carbon can be adjusted. The oxidized carbon-based catalysts exhibit higher activity at lower temperatures compared to untreated carbon, with an optimum oxygen content of around 18%. Increasing the oxygen content and concentration of C-O functionality lowers the catalyst's light-off temperature, offering a potential approach to produce highly active acetylene hydrochlorination catalysts.
Article
Engineering, Chemical
Yutong Pan, Xiaoyu Han, Xiao Chang, Heng Zhang, Xiaohui Zi, Ziwen Hao, Jiyi Chen, Ziji Lin, Maoshuai Li, Xinbin Ma
Summary: Nickel-based catalysts are the most promising selection for CO2 methanation. This study develops ceria-supported bimetallic Ni-Ru catalysts that exhibit high efficiency for low-temperature methanation. The addition of a small amount of Ru to Ni enables intermetallic interaction, enhancing the catalytic capacity for hydrogen activation and CO adsorption, and resulting in a significant increase in the reaction rate for CO2 methanation.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Saisai Wang, Liqi Wan, Chunxiao Jin, Tao Wang, Kaixuan Zhuge, Yuxue Yue, Haiting Cai, Bolin Wang, Renqin Chang, Jia Zhao, Xiaonian Li
Summary: This study proposes a strategy to optimize the electronic structure of Ru single-atom catalysts and applies it to acetylene hydrochlorination. The results demonstrate that the use of appropriate ligands can enhance the performance of the catalysts.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Applied
You Han, Yulian Wang, Yan Wang, Yubing Hu, Yao Nian, Wei Li, Jinli Zhang
Summary: By adding 1-methyl-2-pyrrolidinone (NMP) ligand, the activity and stability of the Cu-pyrrolidone/spherical activated carbon catalysts were significantly improved. The optimal molar ratio of NMP/Cu = 0.25 showed the best performance with a 94.2% acetylene conversion rate. NMP enhanced the dispersion of Cu species, stabilized Cu(+) and Cu(2+) species, and inhibited coke deposition, demonstrating great potential in acetylene hydrochlorination.
APPLIED ORGANOMETALLIC CHEMISTRY
(2021)
Review
Chemistry, Inorganic & Nuclear
Xuxu Wang, Wenqian Chen, Xiaojia Lei, Chao Lei, Nengwu Zhu, Binbin Huang
Summary: Catalytic acetylene hydrochlorination is crucial for the production of vinyl chloride. Using non-mercury catalysts, such as p-block element-regulated catalysts, has gained industrial relevance. Dopant p-block elements can improve catalyst performance and stability, resulting in superior catalytic activity and efficiency.
COORDINATION CHEMISTRY REVIEWS
(2024)
Article
Chemistry, Applied
Jing Li, Lingyun Dai, Yuxi Liu, Jiguang Deng, Lin Jing, Zhiquan Hou, Wenbo Pei, Xing Zhang, Hongxing Dai
Summary: Bimetallic compounds, specifically Ir and IrFex nanocrystals, loaded on mesoporous ceria were studied for their catalytic properties, with 0.59IrFe0.90/mesoCeO2 showing the best acetylene combustion performance. The samples exhibited good water and carbon dioxide resistance, with reversible partial deactivation upon SO2 exposure. The well-dispersed IrFe0.90 NCs and strong interaction with meso-CeO2 were key factors for the excellent catalytic performance.
Article
Chemistry, Physical
Ana Luiza P. Salgado, Felipe C. Araujo, Andre V. H. Soares, Yutao Xing, Fabio B. Passos
Summary: The study investigates Ruthenium-copper bimetallic catalysts supported on modified zirconia for the hydrogenolysis of glycerol to produce 1,2-propanediol. The addition of copper to the Ru-based catalysts resulted in decreased glycerol conversion and increased selectivity to 1,2-propanediol. The best performing catalyst was bimetallic Ru-Cu/m-ZrO2, while catalysts supported on 3%SO4-ZrO2 showed lower activity likely due to sulfur poisoning. Addition of Cu to Ru led to site blockage and tuning of selectivity towards C-O cleavage.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Physical
Jiaqi Yang, Haitao Shen, Xiangqian Yuan, Jigang Zhao
Summary: Gold-based mercury-free catalysts show great potential in the industrial production of vinyl chloride. In this study, the catalytic reaction mechanisms of five sulfur-containing ligand gold-based catalysts were investigated using DFT calculation and DFT-D3 correction. The results revealed that the rate-controlling step in the reaction path is the transfer of proton hydrogen. Valuable theoretical guidance for the preparation of efficient sulfur-containing ligand gold-based catalysts in the future was provided.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2023)
Article
Engineering, Chemical
Shuchun Zhao, Wei Li, Jinli Zhang
Summary: This study utilizes POD and DMD analysis methods to extract the energetical and dynamical characteristics of velocity fields in high-shear mixers using sampling spaces generated through Large-Eddy Simulation. The POD results visualize significant flow structures, while the DMD results reveal the importance of lower frequency flow patterns.
Article
Engineering, Environmental
Junheng Guo, Yudong Liu, Shuchun Zhao, Haojie Li, Wei Li, Jinke Xia, Jiangjiexing Wu, Jinli Zhang
Summary: This article investigates the residence time distribution (RTD) characteristics of high shear mixers (HSMs) through experimental and simulation studies. The results show that adding a distributor or increasing rotor speed improves the local energy dissipation and smoothes the RTD curves. Increasing the number of stator-rotor stages makes the RTD curves closer to plug flow. Higher or thicker rotor-stator teeth favor typical first/second-order reactions. Additionally, correlations between various parameters were obtained, providing useful guidance for the scale-up design and optimization of HSMs.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Hongyang Tian, Houjun Zhang, Jinli Zhang, You Han
Summary: In this study, the nucleation process of nano-iron oxide crystals synthesized via supercritical hydrothermal synthesis was investigated using molecular dynamics with a reactive force field. It was found that high local density areas appeared during the early stages of nucleation, serving as primary candidates for nucleation. Moreover, the amorphous intermediate reorganized through the aggregation and coalescence of prenucleation clusters (PNCs) before the emergence of a crystalline nucleus. The average nucleation rates were observed to generally increase with higher reaction temperatures and system densities, and the volumes of nano-iron oxide clusters remained constant during the simulations.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Biochemistry & Molecular Biology
Jinbo Yang, Xiangxue Cao, Lanfeng Wei, Jianshu Zhang, Jinli Zhang, Ping Liu, Liang Xu, Pengfei Li
Summary: In this study, a four-coordinated organoboron compound, aminoquinoline diarylboron (AQDAB) was used as a photocatalyst for the oxidation of silane to silanol. This method efficiently oxidizes Si-H bonds to form Si-O bonds. The corresponding silanols can be obtained in moderate to good yields at room temperature under oxygen atmospheres, providing a green protocol for the preparation of silanols.
Article
Engineering, Chemical
Shuchun Zhao, Guixuan Shan, Xinhui Yang, Kangkang Ma, Wei Li, Jinli Zhang
Summary: The study investigates the effects of particle size and concentration, rotor revolution speed, and rotor structural parameters on the liquid-liquid extraction process with solid particles. The results show that increasing the rotor revolution speed significantly improves mass transfer performance. The extraction efficiency and mass transfer coefficient increase at low revolution speeds but decrease with higher particle concentration. Larger particle size is detrimental to mass transfer. Additionally, the relationship between the mass transfer coefficient and key parameters is established with high accuracy using machine learning algorithms for HSM design and optimization.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Physical
Tiantong Zhang, Bao Wang, Yao Nian, Menghui Liu, Yiming Jia, Jinli Zhang, You Han
Summary: In this study, the active sites on Cu-based catalysts for acetylene hydrochlorination were investigated. It was found that the indirect ligand-coordinated sites induced by excess copper chloride exhibited superior performance. Molecular dynamics simulation and density functional theory calculations revealed that excess copper chloride molecules spontaneously formed chain structures, leading to the formation of indirect ligand-coordinated sites and electron transfer along the copper chloride chain, which were crucial for the high catalytic activity. These findings provide fundamental insights into the origin of activity and the identification of active sites in Cu-ligand catalysts for acetylene hydrochlorination.
Article
Chemistry, Multidisciplinary
Qiangang Zhang, Haiyang Zhang, Minghui Huang, Zihan Guo, Lijie Yang, Wencai Peng, Jinli Zhang
Summary: A low dispersion and deficiency of active Pt-L1/SAC-IPA catalyst was synthesized using 2-propanol (IPA) solvent and ligand coordination strategy. IPA, with its low boiling point and weak polarity, helps in the dispersion of Pt species. The introduction of phthalimide ligand (L1) modulates the electronic properties of active metals, resulting in the construction of a single-site-dispersed Cl-Pt-N local structure bearing Pt(II) as the active center. The Pt-L1/SAC-IPA catalyst shows enhanced adsorption and activation performances towards HCl, improving its anticoking performance and reducing the reaction energy barrier.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Energy & Fuels
Yuwen Ji, Maolan Xu, Ruili Guo, Wencai Peng, Jianshu Zhang, Jinli Zhang
Summary: In this study, the vacuum evaporation deposition of CuCl catalyst and silicon particles mixture is found to be an effective pretreatment strategy, resulting in excellent catalytic performance of up to 21.2% under the optimum conditions. The vacuum evaporation deposition allows for the uniform deposition of gaseous CuCl on silicon particle surfaces, forming Cu3Si. Moderate temperature and time of the pretreatment promote the growth of copper compounds and shorten the induction period of SiCl4 hydrogenation reaction. The conversion of SiCl4 is positively correlated with the content of Cu3Si, which acts as the active phase exhibiting good catalytic performance.
SOLAR ENERGY MATERIALS AND SOLAR CELLS
(2023)
Editorial Material
Chemistry, Physical
Yao Nian, Xinyuan Huang, Menghui Liu, Jinli Zhang, You Han
Article
Chemistry, Physical
Ye Lv, Mao Peng, Weiwei Yang, Menghui Liu, Aiqun Kong, Yan Fu, Wei Li, Jinli Zhang
Summary: A nickel foam-supported molybdenum dioxide/molybdenum phosphide hybrid electrocatalyst (MoO2/MoP/NF) is reported for highly selective generation of terephthalic acid (TA) via electrocatalytic oxidation (ECO) of p-xylene (PX) in alkaline medium. The MoO2/MoP/NF anode material shows a unique cluster like nanocone architecture, providing abundant active sites for efficient charge transfer kinetics. The synergy between MoO2 and MoP yields high TA selectivity of 94.8% and outstanding faradaic efficiency of 76.9% at a conversion of 71.6%.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Engineering, Environmental
Yifei Wang, Mao Peng, Aiqun Kong, Lin Yang, Jinli Zhang, Jinke Xia, Wei Li
Summary: In this study, a facile procedure was developed to manufacture a superhydrophobic wrinkled skin-covered polypropylene (PP) membrane with excellent separation performance for oil-water emulsions. The prepared membrane showed superior water repellency and high separation efficiency for immiscible oil-water mixtures and water-in-oil emulsions. Furthermore, the membrane exhibited good resistance to solvents and abrasion due to its strong chemical bonding.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Zihan Guo, Wencai Peng, Jian Li, Feng Li, Qiangang Zhang, Lijie Yang, Dongyang Xie, Yanzhao Dong, Jinli Zhang, Haiyang Zhang
Summary: Defect sites and nitrogen species in carbon materials have a direct impact on their catalytic activity for acetylene hydrochlorination. Increasing the density of defect sites often results in a decrease in the content of nitrogen species. In this study, rosette-like nitrogen doped mesoporous carbon materials were synthesized, which have more defect sites than conventional spherical materials. The catalytic performance and nitrogen species analysis showed that pyridine N and pyridinic N+O- are the main active sites. The synergistic effect of defect sites and suitable nitrogen species promotes the reaction process of acetylene hydrochlorination.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Menghui Liu, Chenhui Wang, Zifan Cao, Aiqun Kong, Yusheng Gao, Jinli Zhang, You Han, Wei Li, Yan Fu
Summary: A series of 3D self-standing PtRu/Ni(OH)(2)/NF electrodes were fabricated for electrocatalytic hydrogenation of benzoic acid. The unique coral-shaped architecture of the PtRu/Ni(OH)(2) electrocatalyst possesses excellent charge transfer ability and abundant active sites. The optimized electrode achieved high conversion and selectivity rates for benzoic acid in 0.05 M H2SO4, with a record faradaic efficiency and high performance during multiple cycles.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Rui Duan, Wencai Peng, Jianshu Zhang, Jinli Zhang
Summary: Chlorination of (CH3)2SiHCl/SiHCl3 with metal chlorides (WCl6, MoCl5) was studied to increase the relative volatility and facilitate the distillation process for the removal of carbonaceous impurities from trichlorosilane.
Article
Chemistry, Physical
Hongyang Tian, Houjun Zhang, Jinli Zhang, You Han
Summary: This study investigates nucleation with reactions from supercritical water by using molecular dynamics with a reactive force field. Nano-iron oxide crystals were synthesized via the supercritical hydrothermal synthesis method. The early stages of nucleation showed high local density areas as primary candidates for nucleation. The process involved the formation of amorphous intermediate followed by the emergence of a crystalline nucleus through the aggregation and coalescence of prenucleation clusters (PNCs), deviating from the classical theory of one-step nucleation.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
