Article
Chemistry, Physical
Airi Hirayama, Yuka Tsuchimura, Hiroshi Yoshida, Masato Machida, Shun Nishimura, Kazuo Kato, Keisuke Takahashi, Junya Ohyama
Summary: Cu-CHA zeolites show high catalytic activity in the direct oxidation of CH4 to CH3OH due to their redox properties, particularly the high reducibility of Cu2+ involved in CH4 activation.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Tingyu Liang, Jialing Chen, Sen Wang, Pengfei Wang, Zhangfeng Qin, Fang Jin, Mei Dong, Jianguo Wang, Weibin Fan
Summary: This study investigates the effects of acid density on the methanol-to-hydrocarbon (MTH) performances and deactivation behaviors of H-MCM-22 zeolites. It is found that acid density has a significant impact on MTH performances, while acid distribution has a smaller effect. Increasing acid density promotes hydrogen transfer reactions and the formation of aromatics, ethene, and alkanes. Low acid density results in coke covering acid sites inside the micropores, while high acid density leads to massive coke deposition on the external surface. The deactivation behaviors of H-MCM-22 zeolites can be divided into three stages.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Yida Zhou, Jiani Zhang, Wenyan Ma, Xin Yin, Guangrui Chen, Yinghao Liu, Jiyang Li
Summary: The influence of catalysts on product selectivity in the methanol to olefins (MTO) process was studied in this work. SAPO-14 zeolite catalysts with high selectivity and SAPO-34/SAPO-14 composite zeolite catalysts were successfully synthesized. The results showed that controlling the acidity and pore structure of the catalysts could effectively improve the selectivity for light olefins.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Engineering, Chemical
Chijin Zhang, Kay Lup Andrew Ng, Lixia Yan, Xiang Feng, Binbo Jiang, Zuwei Liao, Jingdai Wang, Yongrong Yang
Summary: The study found that olefin cofeeding during the MTP reaction can significantly increase propylene yield, and recommends using a temperature of 480 degrees Celsius for the HZSM-5 catalyzed MTP process.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Engineering, Environmental
Ling Zhang, Rui Tu, Guoqing Ren, Zhen Li, Shengliang Zhai, Yuchun Xu, Tie Yu
Summary: Optimizing propene selectivity, propene/ethene (P/E) ratio, and catalytic stability in methanol-to-olefin (MTO) research is challenging. A strategy of controlling the acidity of MFI-zeolites through incorporating gallium(III) centers into Silicalite-1 (S-1) is reported. The resultant GaS-1(1.3) zeolite exhibits remarkable propene selectivity, P/E ratio, and catalytic stability, promoting the application of zeolites in sustainable manufacturing of light olefins.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Yanyan Chen, Hongbin Wu, Sen Wang, Dezhi Shi, Mei Dong, Zhangfeng Qin, Jianguo Wang, Weibin Fan
Summary: The co-coupling conversion of propane and methanol is an effective method for the activation of propane. However, the detailed mechanism of this reaction is not fully understood due to its complexity. In this study, density functional theory (DFT) calculations combined with model experiments were conducted to investigate the reaction kinetics and thermodynamics of various elementary steps in propane activation with the assistance of methanol over H-ZSM-5 zeolite. The results revealed that the introduction of methanol significantly reduces the energy barrier for propane activation by generating active intermediates that promote propane dehydrogenation through hydrogen transfer reactions.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
S. Hadi Alaei, Farhad Khorasheh, M. Reza Jafari Nasr, Mehdi Arjmand
Summary: Extensive experimental data were used to develop a comprehensive kinetic model for the methanol to propylene (MTP) process over a ZSM-5 catalyst. Preliminary experiments were performed to determine the reaction conditions that would ensure the absence of external and internal mass transfer resistances. The kinetic experiments were subsequently carried out at 420-500 degrees C under conditions where mass transfer limitations were absent. A detailed reaction network was proposed for the MTP process based on the experimental product distribution and various reported kinetic models in the literature.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Engineering, Chemical
Zhaojun Gao, Qunfei Wang, Tao Yan, Kaiwen Zhao, Wenqi Liu, Qin He, Qiming Sun, Zhongfu Li, Jingyan Zhang, Conghua Liu
Summary: In this study, hierarchically porous SAPO-18 catalysts with abundant intracrystalline mesopores were successfully designed and fabricated. A cost-effective non-surfactant cationic surfactant, PDADMAC, was used as a pore-forming agent, morphology regulator, and silicon inducer. The resulting hierarchical porous SAPO-18 sheets showed improved catalytic performance compared to conventional SAPO-18 zeolite during the methanol-to-olefin reaction.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Xiangkun Wu, Zihao Zhang, Zeyou Pan, Xiaoguo Zhou, Andras Bodi, Patrick Hemberger
Summary: In this study, the experimental detection of methylketene as the precursor of ethylene on HZSM-5 was reported, providing evidence for the computationally predicted ketene-to-ethylene reaction pathway.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Yiou Wang, Enqi Chen, Junwang Tang
Summary: Photocatalytic CO2 conversion to value-added chemicals is a promising solution for current energy and environmental issues, but faces obstacles such as the inertness of CO2 molecule, sluggish multi-electron process, unfavorable thermodynamics, and selectivity control. Despite the challenges, understanding reaction mechanisms and seeking potential solutions are crucial for addressing remaining obstacles in the field.
Article
Engineering, Chemical
Galal A. Nasser, Ali A. Al-Qadri, Anas Karrar Jamil, Idris A. Bakare, Mohammed A. Sanhoob, Oki Muraza, Zain H. Yamani, Toshiyuki Yokoi, Qasim Saleem, Donya Alsewdan
Summary: The study investigated a series of chabazite-based catalysts that facilitate the methanol to olefins reaction, comparing the effects of different treatment methods on their reaction performance. The results showed that the catalyst modified by steam and acid treatment exhibited better stability in the MTO process.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Shanfan Lin, Yuchun Zhi, Wei Chen, Huan Li, Wenna Zhang, Caiyi Lou, Xinqiang Wu, Shu Zeng, Shutao Xu, Jianping Xiao, Anmin Zheng, Yingxu Wei, Zhongmin Liu
Summary: The study reveals the complete theoretical picture of the autocatalytic reaction network occurring on HZSM-5 zeolite, which facilitates catalyst design and process control for methanol-to-hydrocarbons technology.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Applied
Mengheng Wang, Jincan Kang, Xuewei Xiong, Fuyong Zhang, Kang Cheng, Qinghong Zhang, Ye Wang
Summary: Recent studies show that bifunctional catalysts of metal oxides and zeolites can control hydrocarbon distribution in syngas conversion. SAPO zeolites' micropore window size primarily determines the distribution, while cage size and reaction conditions only affect it within a narrow range of chain length. Zeolite topology has a similar impact on hydrocarbon distribution in syngas conversion compared to methanol conversion.
Article
Materials Science, Multidisciplinary
Mehran Sajad, Yuyan Zhang, Martin Kubu, Michal Mazur, Roman Bulanek, Jiri Cejka
Summary: In this study, well-dispersed Pd nanoparticles were encapsulated within IPC-2 and IPC-4 zeolites using the ADOR process. The Pd@IPC-2 and Pd@IPC-4 showed higher catalytic activity than Pd/IPC-2 and Pd/IPC-4 in the direct dehydrogenation of propane. The size of zeolite channels and the structure of the framework strongly influenced the catalytic activity.
APPLIED MATERIALS TODAY
(2022)
Article
Chemistry, Physical
Hegen Zhou, Hua Jin, Yanli Li, Yi Li, Shuping Huang, Wei Lin, Wenkai Chen, Yongfan Zhang
Summary: The adsorption and hydrogenation of carbon dioxide on gamma-Al2O3(110) surface-supported copper clusters of different sizes were studied using density functional theory calculations. It was found that CO2 activation was more pronounced at the partially hydroxyl-covered interface. The catalytic mechanisms of CO2 conversion to methanol were explored, and the formate pathway was identified as the preferred reaction pathway. However, surface hydroxylation had a negative effect on the catalytic activity in CO2 conversion.
Review
Nanoscience & Nanotechnology
Shuangchao Zhao, Keyan Li, Jiaming Wu, Jiaxing Zhang, Xiangyang Li, Xinwen Guo, Chunshan Song
Summary: This study successfully improved the efficiency of photocatalytic CO2 reduction by fabricating a tubular In2O3-C/CdIn2S4 (IOC/CIS) ternary heterojunction. The introduction of carbon accelerated charge migration, enhanced light absorption, and CO2 adsorption. The resulting 5IOC/CIS sample exhibited significantly improved activity.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Chemical
Mengjiao Pei, Keyan Li, Xiangyang Li, Chunshan Song, Xinwen Guo
Summary: Iron phthalocyanine/carbon nitride (FePc/CN) hetero-junction nanosheets were prepared using calcination method and exhibited excellent activation of peroxydisulfate (PDS) for tetracycline (TC) degradation under visible light. The FePc/CN-6 heterojunction showed significant improvement in degradation rate compared to CN and FePc due to the synergistic effect of photocatalysis and PDS activation. The construction of intimate interface via pi-pi conjugation enhanced charge separation and transfer, resulting in enhanced PDS activation and photodegradation.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Review
Chemistry, Physical
Haiyan Wang, Yanan Diao, Zirui Gao, Kevin J. Smith, Xinwen Guo, Ding Ma, Chuan Shi
Summary: This review highlights the applications and challenges of transition-metal carbides in methane reforming reactions (MRRs) and discusses strategies to improve their performance. The findings provide guidance for the future design of efficient catalysts for hydrogen production.
Article
Chemistry, Multidisciplinary
Jun Du, Hainan Shi, Jiaming Wu, Keyan Li, Chunshan Song, Xinwen Guo
Summary: This study presents an ingenious calcination strategy to introduce sulfur vacancies and enhance the interfacial interaction in a TiO2@ZnIn2S4 heterojunction, greatly improving the photocatalytic CO2 reduction activity.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Yanli Wang, Hong Yang, Yi Zuo, Dongxu Tian, Guangjin Hou, Yaqiong Su, Zhaochi Feng, Xinwen Guo, Can Li
Summary: In this study, we identified two new titanium sites in the environmentally friendly titanium-containing zeolite catalyst, TS-1. These sites, namely penta-coordinated Ti(OH)2(OSi)3 and hexacoordinated Ti(OH)4(OSi)2, were characterized using UV resonance Raman spectroscopy and density functional theory calculations. The hexacoordinated Ti(OH)4(OSi)2 site exhibited higher catalytic activity compared to the penta-coordinated Ti(OH)2(OSi)3. Additionally, the catalytic activity of Ti(OH)4(OSi)2 was found to be approximately 8.7 times higher than that of the known tetra-coordinated framework Ti(OSi)4 sites, indicating its high activity in propylene epoxidation to propylene oxide.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Shujie Shang, Limin Ren, Quanjie Liu, Ajuan Zhou, Jiaxing Zhang, Bangjian Liu, Anfeng Zhang, Xinwen Guo
Summary: Ultrafast synthesis of nanocrystal assembled ZSM-48 spheres and regulation of acidity were achieved in just 1.5 hours using a pretreated-seed-solution-assisted strategy. The resulting product demonstrated excellent performance as an acid support in hydroconversion reactions of long-chain alkanes. By altering the introduction sequence of aluminum source, it was found that the crystallization behavior and acid properties of the ZSM-48 zeolite varied significantly, leading to differences in catalytic activity and selectivity for n-C-12 hydroisomerization.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Engineering, Chemical
Fei Yuan, Guanghui Zhang, Mingrui Wang, Jie Zhu, Miao Zhang, Fanshu Ding, Zening Cheng, Chunshan Song, Xinwen Guo
Summary: This study reports a series of Fe-Co bimetallic catalysts derived from Fe-Co-Mg layered double hydroxides (LDHs) with different Fe/Co ratios for converting CO2 to light olefins. The best catalyst, FeCo-9:1-LDH, showed a high selectivity of C-2-C-4(=) over 36% at a CO2 conversion higher than 40%. The catalyst can be carburized to Co-modified iron carbide (Fe5C2), which exhibits higher CO2 conversion and C-2-C-4(=) selectivity compared to the catalyst prepared by impregnating Co and Fe onto MgO support.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Biotechnology & Applied Microbiology
Jiaming Wu, Hainan Shi, Keyan Li, Xinwen Guo
Summary: Single-atom catalysts (SACs) have great potential in environmental catalysis due to their high atomic utilization efficiency, unique metal coordination structure, and metal-support interactions. As single-atom catalysis progresses into dual-atom catalysts, the introduction of more complex active sites and synergistic interactions presents new opportunities and challenges in heterogeneous catalysis. This review summarizes the current advantages of SACs and their applications in environmental catalysis, discusses the issues of stability and large-scale production, and provides an outlook on the future development of single-atom catalysis.
CURRENT OPINION IN CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Applied
Jing Yue, Junjie Li, Min Liu, Wen Liu, Xiujie Li, Sujuan Xie, Chunshan Song, Xinwen Guo, Xiangxue Zhu
Summary: In this study, high-silica MFI zeolite was successfully prepared using a low-temperature crystallization method and seed-directed and C2H5OH filling techniques. The synthetic gel was purified to exclude impurity phases, and well-crystallized ZSM-5 samples with controllable Si/Al ratios and uniform particle sizes were obtained. The obtained high-silica MFI zeolite exhibited superior catalytic stability compared to the conventional sample during methanol-to-propylene and n-butene cracking reactions.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Xiangyang Li, Jiaming Wu, Sufeng An, Keyan Li, Jiaxing Zhang, Mengjiao Pei, Chunshan Song, Xinwen Guo
Summary: We propose a simple bottom-up strategy for preparing crystalline polymeric carbon nitride (CCN) with ultrathin 2D nanosheet structures. CCN can efficiently remove various high-concentration organic pollutants and heavy metal ions under visible light irradiation. It also exhibits outstanding photocatalytic performance in the water-splitting reaction. The highly boosted activity of CCN is attributed to the significantly improved charge separation, increased active sites, and enhanced visible light absorption.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Xiaoyu He, Yujia Ding, Zhennan Huang, Min Liu, Miaofang Chi, Zili Wu, Carlo U. Segre, Chunshan Song, Xiang Wang, Xinwen Guo
Summary: A photocatalyst TiO2/Ti-BPDC-Pt with a self-grown TiO2/Ti-MOF heterojunction, selectively anchored high-density Pt single-atomic cocatalysts on Ti-BPDC, achieves photocatalytic hydrogen evolution. The intimate heterojunction efficiently separates electrons and holes in a direct Z-scheme, and Pt is selectively anchored on Ti-BPDC in the form of single atoms. The tailored TiO2/Ti-BPDC-Pt exhibits significantly enhanced activity compared to other TiO2- or MOF-based catalysts, showing the importance of the balance of two simultaneously exposed domains of heterojunctions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Mengnan Sun, Xiaowa Nie, Xinwei Zhang, Sirui Liu, Chunshan Song, Xinwen Guo
Summary: The potential roles of introducing methanol and the mechanism of methane-methanol coupling were investigated using density functional theory (DFT) calculations. The results show that Zn/ZSM-5 catalyst exhibits superior activity for both reactant activation and C-C coupling. Co, Ni, or Pd can be added to Zn/ZSM-5 to further enhance the reaction.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Tianlong Wang, Wei Huang, He Han, Jiaxing Zhang, Huifang Wu, Xin Yan, Yuanjuan Jiang, Lu Fang, Bochun Zhang, Xinwen Guo, Limin Ren
Summary: A facile hydrothermal etching-healing strategy is proposed to fabricate Sn-MWW zeolite without using any supporting agents and additives. This approach has the advantages of low organic structure-directing agent consumption and rapid growth, resulting in successful Sn introduction and excellent catalytic performance.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Inorganic & Nuclear
He Han, Hong Yang, Anfeng Zhang, Limin Ren, Xiaowa Nie, Chaoqiu Chen, Min Liu, Chuan Shi, Chunshan Song, Xinwen Guo
Summary: Applying consecutive SiO2-P2O5-MgO (SPM) and SiO2 surface coatings on ZSM-5 catalysts can achieve high para-selectivity, while loading Pt, Ni, and (Pt+Ni) metals can enhance catalytic stability. The study confirms that the most effective location for metal loading is on the external surface of the modified catalysts.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Multidisciplinary
Xiangyang Li, Keyan Li, Jun Du, Mengjiao Pei, Chunshan Song, Xinwen Guo
Summary: In this study, nitrogen-rich porous polymeric carbon nitride was prepared and showed superior photocatalytic performance for the degradation of various high concentration organic pollutants. The outstanding performance can be attributed to the rich amino defects and porous structure.
ENVIRONMENTAL SCIENCE-NANO
(2022)
Article
Chemistry, Physical
Zi-Ye Liu, Qian-Yu Wang, Ji-Ming Hu
Summary: In this study, a layered carbon dot composite catalyst (NiFe LDH@CDs) was prepared using a one-step coprecipitation method, without the need for heating or hydrothermal treatment. The CD-functionalized catalyst facilitated rapid charge transfer and accelerated the oxygen evolution reaction. Additionally, the heterojunction structure formed between NiFe LDH and CDs efficiently suppressed photoelectron-hole recombination.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Rohit Kumar, Ankit Kumar Srivastava, Palaniyappan Nagarasu, Vedichi Madhu, Ekambaram Balaraman
Summary: We designed and synthesized a NN-CoII bidentate complex and used it for the amination of alcohols under mild and solventless conditions. The complex exhibited good reactivity towards both primary and sterically hindered secondary alcohols, providing high yields of amines. The pyrazole moiety in the ligand played a crucial role in the reaction. Furthermore, we demonstrated the reusability of the complex as a homogeneous cobalt catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shivanand Chettri, Liang-Ting Wu, Sagarmani Rasaily, Debesh Sharma, Bikram Gurung, Rajani Dewan, Sudarsan Tamang, Jyh-Chiang Jiang, Anand Pariyar
Summary: Replicating the enzymatic surface microenvironment in vitro is challenging, but constructing an analogous model could facilitate our understanding of surface effects and aid in developing an efficient bioinspired catalytic system. In this study, five unique Cu2O morphologies were generated, and the surface morphology variations were found to be a consequence of differences in the exposure of low-index facets. The reactivity of Cu2O was found to be influenced by the proportion of {110} planes, with r-Cu2O exhibiting the highest reactivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Yong Tang, Jianhao Qiu, Dingliang Dai, Guanglu Xia, Lu Zhang, Jianfeng Yao
Summary: Defect engineering has been shown to improve the photocatalytic performance. This study investigated the use of defect-rich UiO-66-NH2 wrapped by ZnIn2S4 as a catalyst for photocatalytic H2O2 production. The defects in UiO-66-NH2 enhanced O-2 adsorption and charge separation, leading to higher H2O2 yield. The insights from this work can advance the research in defect engineering of MOFs and photocatalytic H2O2 synthesis.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Ruiyang Qu, Shuxin Mao, Jana Weiss, Vita A. Kondratenko, Evgenii V. Kondratenko, Stephan Bartling, Haifeng Qi, Annette-Enrica Surkus, Kathrin Junge, Matthias Beller
Summary: The hydrogenation of amides, a challenging reaction usually performed at high temperatures, has been achieved under milder conditions using a new Pt-MoOx/TiO2 catalyst. This catalyst system enables the selective hydrogenation of various amides and imides.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Xiaoran Niu, Ao Wang, Lei Tong, Lei Wang, Yuan Kong, Chenliang Su, Hai-Wei Liang
Summary: This study introduces a novel intermetallic PdCu3 catalyst supported on defective nanodiamond-graphene (ND@G), which exhibits high selectivity (95%) and remarkable activity (turnover frequency: 2940 h(-1)), six times higher than that of the commercial Lindlar catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Review
Chemistry, Physical
Zhiyuan Zheng, Yiming Yue, Hongying Zhuo, Qinggang Liu, Yanqiang Huang
Summary: This review presents the recent research advances on single-atom catalysis for deep reduction of CO2. Detailed introductions and summaries were classified into three categories based on proton-coupled multi-electron transfer approaches: strengthening metal-support interaction, rational design and regulation of coordination environment, and development of SACs with multi-atom active sites. The challenges and future research directions in the field of SACs for CO2 reduction are also proposed.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shiv Kumar, Paramita Datta, Anup Bhunia, Swadhin K. Mandal
Summary: This article reports a transition-metal-free process for in situ denitrogenation of tosylhydrazones, resulting in the production of various sulfones. The authors used a phenalenyl-based odd alternant hydrocarbon as a photoredox catalyst, which acted as a potent oxidant to facilitate the denitrogenation reaction. The method showed wide functional-group tolerance and high yields, making it suitable for late-stage modification of natural products.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
L. A. Luque-Alvarez, J. Gonzalez-Arias, F. Romero-Sarria, T. R. Reina, L. F. Bobadilla, J. A. Odriozola
Summary: Currently, the production of acetic acid through the carbonylation reaction of methanol has limitations, leading to the exploration of alternative methods using heterogeneous catalysts. This study investigates the methanol carbonylation reaction over a Cu-H-MOR catalyst and proposes a reaction mechanism based on the catalytic behavior and performance of the catalyst. The results provide insights into the reaction mechanism and the involvement of acid and redox centers.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)