Article
Chemistry, Physical
Xinqiang Feng, Ziheng Cui, Yufei Bao, Haodong Chu, Xue Wu, Chun Shen, Tianwei Tan
Summary: In this study, a series of metal phosphate catalysts with varied acid strength were prepared to investigate their role in the reaction between DMF and HDO. Strong acid sites were found to play a vital role in the further condensation of HDO, leading to a decrease in PX selectivity. The study provides insights into the importance of acid strength for rational design of new catalysts and mechanistic understanding.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Yi Zhao, Kai-Zhi Wang, Ze-Hui Sun, Qi Zhang, Zi-Jian Wang, Yong-Mei Liu, He-Yong He, Yong Cao
Summary: The dispersion of NbOx on the inner surface of MCM-type mesoporous silica as a catalyst enables efficient production of PX from concentrated DMF. This catalyst exhibits excellent activity, selectivity, and stability, highlighting its importance in the conversion of DMF and related furanic compounds to aromatic products.
Article
Chemistry, Physical
Ferdy J. A. G. Coumans, Ezgi Demiroz, Nikolay Kosinov, Emiel J. M. Hensen
Summary: This study investigates the potential of amorphous silica-alumina (ASA) as a substitute for zeolites in the synthesis of p-xylene through Diels-Alder cycloaddition (DAC) of ethylene to 2,5-dimethylfuran (2,5-DMF). ASA shows promising yields of p-xylene and Bronsted acid sites (BAS) are identified as the active sites for the reaction. Additionally, ASA proves to be a more effective catalyst than zeolite after calcination-regeneration treatment.
Article
Chemistry, Physical
Chengming Wu, Ting Wu, Jifan Li, Chun-Ling Liu, Wen-Sheng Dong
Summary: A series of zirconium phosphates (ZrP-x) with various P/Zr ratios were prepared and showed excellent catalytic performance in the synthesis of p-xylene (PX) from 2,5-dimethylfuran (DMF) and ethylene. The catalyst ZrP-2.5 exhibited a high PX yield of 89.2% and a productivity of 72.3 mmol(PX).g(cat)(-1).h(-1) at 250 degrees C with a small amount of catalyst. The excellent catalytic performance was attributed to the synergy between acidic sites, balanced acidity, and abundant mesopores.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Physical
Christopher Sauer, Anders Loren, Andreas Schaefer, Per-Anders Carlsson
Summary: The valorization of 2,5-dimethylfuran (2,5-DMF) through catalytic fast pyrolysis (CFP) was studied using on-line FTIR-MS gas phase analysis. The selectivity towards benzene, toluene, and xylene (BTX) aromatics decreased with time on stream (TOS), while the isomerization rates of 2,5-DMF towards 2,4-dimethylfuran and cyclic ketones increased, indicating the involvement of specific active sites.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Review
Energy & Fuels
Saikat Dutta, Navya Subray Bhat
Summary: This work reviews the renewable synthesis of p-xylene from biomass-derived carbohydrates, discussing the techno-economic analysis of renewable PET and the possibility of a circular economy using chemical and enzymatic recycling strategies. The article also summarizes the role and influencing factors of catalysts in the synthesis of PX.
BIOMASS CONVERSION AND BIOREFINERY
(2023)
Article
Green & Sustainable Science & Technology
Yixuan Yu, Huai Liu, Junhua Zhang, Heng Zhang, Yong Sun, Lincai Peng
Summary: We constructed amorphous bimetal Ni-Fe borides as efficient catalysts for the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural (HMF) into 2,5-dimethylfuran (DMF), a potential biofuel candidate. The Ni(1.52Fe0.36)BOx catalyst achieved a near-quantitative DMF yield under mild operating conditions, with an excellent DMF formation rate that is significantly higher than state-of-the-art nickel-based catalysts. Mechanistic investigations revealed that the presence of Fe contributed to the generation of electron-enriched metal sites and powerful acidic sites, promoting the hydrogen activation and cleavage of C-O bond. The Ni(1.52Fe0.36)BOx catalyst also showed good recyclability and universality in the hydrogenolysis of various biomass-derived unsaturated aldehydes.
Article
Chemistry, Applied
Duozheng Ma, Xiangcheng Li, Chuang Liu, Caroline Versluis, Yingchun Ye, Zhendong Wang, Eelco T. C. Vogt, Bert M. Weckhuysen, Weimin Yang
Summary: Zeolites have played important roles in industrial catalysis, but have shown limited efficiency in the conversion or production of bioderived chemicals. In this study, a new aluminosilicate zeolite named SCM-36 was synthesized, which showed better catalytic performance and recyclability.
CHINESE JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Jyun-Yi Yeh, Season S. Chen, Shih-Cheng Li, Celine H. Chen, Tetsuya Shishido, Daniel C. W. Tsang, Yusuke Yamauchi, Yi-Pei Li, Kevin C-W Wu
Summary: The heterogeneous metal-organic framework Bi-BTC efficiently catalyzed the synthesis of para-xylene from bio-based 2,5-dimethylfuran and acrylic acid with a promising yield of 92%, under relatively mild conditions (160 degrees C, 10 bar), and exhibited a low reaction-energy barrier of 47.3 kJ mol(-1). The proposed reaction strategy also shows remarkable versatility for furan derivatives such as furan and 2-methylfuran.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Rongrong Zhao, Shikun Li, Lixin Bi, Qiang Fu, Hongzi Tan, Ming Wang, Hongyou Cui
Summary: A renewable synthesis of p-xylene (PX) using biomass-derived 2,5-dimethylfuran (2,5-DMF) and ethanol was achieved through the Diels-Alder cycloaddition reaction. Catalyst selection and modification greatly influenced the product distribution and reaction performance.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Zhanghui Xia, Libo Niu, Yadan An, Gang Bian, Tianming Li, Guoyi Bai
Summary: A ternary Ni-Al/CoOx-1 catalyst was prepared, which showed high efficiency in synthesizing 2,5-dimethylfuran under mild reaction conditions. The addition of Al improved the stability of the structure and promoted electron transfer, enhancing the catalytic activity.
Article
Chemistry, Multidisciplinary
Haodong Chu, Xinqiang Feng, Xue Wu, Jianting Song, Chun Shen, Tianwei Tan
Summary: The efficient and green conversion of cellulose into p-xylene (PX) is important for utilizing biomass wastes and promoting the recycling economy. A new two-step PX production route via 2,5-hexanedione (HDO) has been proposed, simplifying the process and reducing costs. The highest yields of 64% and 85% were achieved for HDO/2,5-dimethylfuran (DMF) and PX during the first and second steps, respectively.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Anh Tuan Hoang, Ashok Pandey, Zuohua Huang, Rafael Luque, Kim Hoong Ng, Agis M. Papadopoulos, Wei-Hsin Chen, Sakthivel Rajamohan, H. Hadiyanto, Xuan Phuong Nguyen, Van Viet Pham
Summary: This review discusses the potential and methods of catalytic transformation of waste carbohydrates into 2,5-dimethylfuran (DMF) as a renewable fuel. The significant catalysts, DMF production mechanisms, reaction conditions, and other key factors affecting DMF yield are summarized. Furthermore, the purification process, commercialization potential, and economic feasibility of DMF production are explored, with insightful future directions identified.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Ferdy J. A. G. Coumans, Aleksei Bolshakov, Rim C. J. van de Poll, Dimitra Anastasiadou, Brahim Mezari, Emiel J. M. Hensen
Summary: A variety of methods were used to synthesize amorphous silica-alumina (ASA) and investigate the role of aluminum species and surface area in catalytic reactions. The study found that Bronsted acidity is crucial for p-xylene formation.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Energy & Fuels
Martyna Przydacz, Marcin Jedrzejczyk, Jacek Rogowski, Dris Ihiawakrim, Nicolas Keller, Agnieszka M. Ruppert
Summary: The establishment of future biorefinery schemes requires the conversion of renewable bioresources into eco-friendly fuels and chemicals. The use of bimetallic NiFe alloys supported on TiO2 as catalysts allows for the high-yield production of 2,5-dimethylfuran (DMF), a potential biofuel competitor to ethanol. The preparation method and reduction temperature of the catalyst are crucial for achieving the desired structure and behavior, with a core/shell structure of the NiFe alloy being the key to high performance.
Article
Chemistry, Physical
Dongyang Zhang, Jianbo Zhang, Run Li, Huiyong Chen, Qingqing Hao, Yonghui Bai, Jianxuan Shang, Lei Zhang, Xiaoxun Ma
Summary: This study investigates the effects of thermal treatment temperature and nickel nitrate impregnation concentration on the CO2 methanation reaction using commercially available coal char supported nickel catalysts.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Lei Tao, Poom Sittisomwong, Bingyuan Ma, Anyang Hu, Dawei Xia, Sooyeon Hwang, Haibo Huang, Peng Bai, Feng Lin
Summary: Free-standing carbon nanofiber films with controllable crystallinity and surface chemistry are used to investigate the correlation between Na+ reaction kinetics, storage mechanism, and electrolyte environment. The ion solvation effect and solid-electrolyte interphase (SEI) properties determine the kinetics and storage mechanism. By tuning the SEI chemistries, high initial Coulombic efficiency, ultra-long cycle life under fast charging, and excellent low-temperature performance can be achieved.
ENERGY STORAGE MATERIALS
(2023)
Article
Engineering, Environmental
Wen-Hui Hu, Meng-Nan Liu, Qun-Xing Luo, Jianbo Zhang, Huiyong Chen, Long Xu, Ming Sun, Xiaoxun Ma, Qing-Qing Hao
Summary: This study investigates the influence of microscale structure of MWW zeolites on the kinetics for acylation of anisole with acetic anhydride. It is found that the acylation reaction occurs solely on the external acid sites of MWW zeolites, and the single-layer MWW (SL-MWW) exhibits higher recycle stability compared to the multiple-layer MWW (ML-MWW). The confinement effect within 12MR pockets on the surface of SL-MWW results in difficult desorption of product and small rate constant.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Chemical
Yuchen Yuan, Huihui Ping, Dennis T. Lee, Peter Corkery, Zhen Zhang, Cui Liu, Shuang-mei Xue, Liwei Zhuang, Michael Tsapatsis
Summary: In this study, a detailed computational fluid dynamics (CFD) model of the atomic layer deposition (ALD) feeding system has been developed and validated, which considers the roles of ALD valves and manifolds. Numerical simulations were conducted to accurately predict the dosing amounts and spatiotemporal distributions of the precursors, and the results were validated by experimental data. The operating flexibility of the feeding system was examined by simulating different precursors, operating conditions, and structures of the feeding system.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Applied
Junshan Zhang, Jianbo Zhang, Panpan Jiang, Jianxuan Shang, Jianyou Wang, Huiyong Chen, Qingqing Hao, Lei Zhang, Xiaoxun Ma
Summary: The effects of CO2 gasification conditions on the surface metal species, pore structures and morphology of transition metal oxide/carbon hybrid materials were investigated. The as-prepared hybrid materials show good electrochemical performance, with specific capacitance up to 369.5-750.6 F g(-1) and energy density of 13.9 Wh kg(-1). Excellent cycling performance was also achieved.
JOURNAL OF POROUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Guangyue Xu, Xiang Zhang, Zhuoya Dong, Wanying Liang, Tianci Xiao, Huiyong Chen, Yanhang Ma, Yang Pan, Yao Fu
Summary: In this study, a ferric catalyst confined in a zeolite framework was synthesized, which exhibited high selectivity and stability, and showed resistance to coking.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Anne V. Le, Biplab Rajbanshi, Raul F. Lobo, Peng Bai
Summary: In this study, DFT calculations were used to investigate the mechanisms of propene metathesis catalyzed by WOx/SiO2. The results showed that there are still many mechanisms of heterogeneous catalyzed metathesis reactions that are not well understood. The pseudo-Wittig mechanism was found to be the most favorable method for generating initial alkylidene active sites. The allylic and vinylic C-H activations are more difficult and require the reduction of surface sites to W(+4).
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Ajibola Lawal, Omar A. Abdelrahman
Summary: The spatial distribution of tetrahedrally coordinated aluminum in zeolite was investigated using the Hofmann elimination reaction of alkylamine as a probe. The stability of the adsorbed alkylammonium was found to be crucial for accurate estimation of isolated protons. N-propylamine was shown to be an appropriate probe molecule for quantifying isolated protonic sites on zeolite surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Qiang Luo, Hanyi Duan, Michael C. McLaughlin, Kecheng Wei, Joseph Tapia, Joseph A. Adewuyi, Seth Shuster, Maham Liaqat, Steven Suib, Gael Ung, Peng Bai, Shouheng Sun, Jie He
Summary: We used polymer N-heterocyclic carbenes (NHCs) to control the microenvironment surrounding metal nanocatalysts, enhancing their catalytic performance in CO2 electroreduction. Three polymer NHC ligands were designed with different hydrophobicity: hydrophilic poly(ethylene oxide) (PEO-NHC), hydrophobic polystyrene (PS-NHC), and amphiphilic block copolymer (PEO-b-PS-NHC). The introduction of hydrophobic PS segments led to a twofold increase in the partial current density for CO formation. The hydrophobic polymers altered the hydrogen bonding structures of water, improving CO2 diffusion and subsequent reduction.
Article
Chemistry, Physical
Yachan Liu, Gustavo Perez, Zezhou Cheng, Aaron Sun, Samuel C. Hoover, Wei Fan, Subhransu Maji, Peng Bai
Summary: Zeolites are widely used in the chemical industry due to their selective adsorption and reaction capabilities. ZeoNet is a representation learning framework that uses convolutional neural networks and 3D volumetric representations for predicting zeolite adsorption. It achieves high accuracy and efficiency in its predictions.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Inorganic & Nuclear
Daizong Han, Dongyuan Yang, Chenyao Bi, Guoqing Zhang, Fei Yang, Qingqing Hao, Jianbo Zhang, Huiyong Chen, Xiaoxun Ma
Summary: A fast and efficient synthesis strategy for highly crystalline SAPO-14 via dry-gel conversion is showcased, shortening the crystallization time to 8 hours and increasing the product yield to 71.6% compared to the conventional hydrothermal synthesis. The SAPO-14 produced by this method exhibits superior catalytic performance and is a promising catalyst candidate for the selective conversion of methanol to propylene.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Shubham Malviya, Peng Bai
Summary: In this study, a computational procedure for capturing the configuration changes of transition states in the specific environment of catalyst pore walls was developed. The method estimated the transition state entropy by the number of accessible transition state configurations at each active site. The resulting site-dependent transition state energetics allowed the calculation of ensemble-averaged activation barriers. The protolytic cracking of n-butane in different zeolites was then studied using this approach.
Article
Chemistry, Physical
Bing Wang, RuiQing Zhang, Zhuo Li, ChuanHui Shi, EnZhou Liu, Zheng Zheng, Bo Zhou, MengTing Ji, HuiYong Chen
Summary: This study demonstrates the successful construction of a hybrid van der Waals heterostructure consisting of 3D supramolecular networks and 2D semiconductor Ag3PO4, which exhibits significantly enhanced photocatalytic degradation efficiency and stability. The mechanism and charge transfer behavior were revealed through molecular dynamics simulations and experimental analysis.
APPLIED SURFACE SCIENCE
(2023)
Review
Chemistry, Applied
Wei Wang, Lei He, Qunxing Luo, Linyang Wang, Jing Wang, Huiyong Chen, Zongcheng Miao, Qiuxiang Yao, Ming Sun
Summary: Research on the synthesis of zeolite molecular sieves focuses on manipulating their properties by adjusting particle size, composition, and morphology. The core and shell concept particles, which integrate multiple functions into a single shape, have been extensively studied. This article presents novel design strategies for zeolite-related core and shell concept particles and their application in conventional thermal catalysis.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Engineering, Environmental
Xin Yang, En Yang, Bo Hu, Jiahui Yan, Fangna Shangguan, Qingqing Hao, Huiyong Chen, Jianbo Zhang, Xiaoxun Ma
Summary: This paper proposes a method for the confined growth of Ni(OH)(2) nanosheets within three dimensionally ordered mesoporous carbon (3DOMC) by steam-assisted crystallization. The resulting composite material exhibits high crystallinity and can be reduced to highly segregative Ni nanoparticles. The Ni/3DOMC catalyst shows superior catalytic performance in methane decomposition, with higher methane conversion and hydrogen output rate, as well as better catalytic stability.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
