Article
Engineering, Environmental
Jian Zhu, Guofeng Zhao, Chao Meng, Pengjing Chen, Xue-Rong Shi, Yong Lu
Summary: A high-performance InNi3C0.5/Ni-foam catalyst has been developed for the gas-phase hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The catalyst exhibits a high turnover frequency of 636 h(-1) and effectively activates DMO while hindering over-hydrogenation of EG to ethanol. This catalyst shows promising potential for industrial applications with full DMO conversion and high EG selectivity.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Fakhrony Sholahudin Rohman, Syed Hussaini Syed Sulaiman, Norashid Aziz
Summary: The study focused on utilizing a copper-based catalyst for gas-phase dimethyl oxalate hydrogenation to produce ethylene glycol, achieving optimal conversion, selectivity, and yield through simulation software and multivariable optimization.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Xianlong Gao, Guoqing Zhao, Lei Miao, Lei Li, Zhirong Zhu
Summary: In this study, a series of Cu-ZnO-ZrO2-La2O3 catalysts were synthesized for DMA hydrogenation, and it was found that the CZZ-L2-CP catalyst exhibited the highest catalytic activity. This is attributed to the presence of more oxygen vacancies, decreased electron density of surface La2O3 species, and the electron donor-acceptor interaction between lanthanum and copper species, which prevented the formation of larger copper particles.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Xiaoguang San, Xiaohui Gong, Yiming Lu, Juhua Xu, Liming He, Dan Meng, Guosheng Wang, Jian Qi, Quan Jin
Summary: In this study, a novel MOF-derived Cu/SiO2 catalyst was developed for the hydrogenation of DMO to EG. The catalyst showed high catalytic activity and stability, with a controllable distribution of Cu active sites. Compared to traditional catalysts, the MOF-CmS catalyst exhibited higher catalytic activity.
Article
Chemistry, Applied
Gianfranco Giorgianni, Chalachew Mebrahtu, Siglinda Perathoner, Gabriele Centi, Salvatore Abate
Summary: Cu/SiO2 catalysts prepared by the deposition-decomposition (DD) method using ammonium hydroxide and pre-reduced in pure hydrogen show improved ethylene glycol (EG) yields and stability.
Article
Biotechnology & Applied Microbiology
Xiangpeng Kong, Ruihan Wu, Peihong Yuan, Yuehuan Wu, Ruihong Wang, Xiliang Chang, Man Wang, Xiaoyu Wang, Jiangang Chen
Summary: Cu-doped CoCu/ZnO catalysts were successfully synthesized and applied to the selective hydrogenation of syngas-derived dimethyl oxalate (DMO) to produce ethylene glycol (EG). The Cu content significantly influenced the properties and structures of the catalysts. The CoCu20/ZnO catalyst with 20.0 wt% Cu additive exhibited the highest DMO conversion and EG yield, and showed excellent thermal stability.
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Xiangpeng Kong, Xinming You, Peihong Yuan, Man Wang, Yuehuan Wu, Ruihong Wang, Jiangang Chen
Summary: In this study, Cu catalysts reinforced by Al3+ dopants with different chemical features were successfully synthesized, and the structure evolution and interface effect were explored. The results showed that the choice of precipitants during precursor preparation significantly affected the chemical form of Al3+ and Cu/Al bonding. The CuAl catalyst achieved high ethylene glycol and ethanol yields in DMO hydrogenation. The presence of surface Cu+ sites and Cu-O-Al patterns played important roles in the catalytic behavior, with CuAl(O) catalyst exhibiting enhanced catalytic stability.
Article
Chemistry, Physical
Deliang Yang, Ling Lin, Rong Guo, Peiyu Zhao, Wei Cheng, Wenpeng Yuan, Yeyan Qin, Yuangen Yao
Summary: The study shows that different silver promotion methods have significant effects on the activity, selectivity, and stability of Cu-Ag/SiO2 catalysts. Introducing silver promoter through impregnation method B can enhance the activity and selectivity of the catalyst, as well as improve the stability of the Cu/SiO2 catalyst.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Deliang Yang, Runping Ye, Ling Lin, Rong Guo, Peiyu Zhao, Yanchao Yin, Wei Cheng, Wenpeng Yuan, Yuangen Yao
Summary: Boron (B) promoter modified Cu/SiO2 bifunctional catalysts were synthesized and used for efficient hydrogenation of dimethyl oxalate to produce ethylene glycol and ethanol. The boron promoter significantly improved the catalyst performance by enhancing structural characteristics. The optimized catalyst exhibited excellent low temperature catalytic activity and long-term stability, maintaining high selectivity for ethylene glycol and ethanol.
Article
Chemistry, Physical
Xiangpeng Kong, Yuehuan Wu, Peihong Yuan, Man Wang, Peng Wu, Lifeng Ding, Ruihong Wang, Jiangang Chen
Summary: The synthesis of Al2O3 doped mesoporous monometallic Cu catalysts was achieved through the thermal decomposing of the self-assembly Cu species derived from the oxalate precursor. The calcination temperature during catalyst preparation was found to significantly influence the textural and surface properties of the CuAl catalysts, ultimately determining their catalytic behavior in dimethyl oxalate (DMO) hydrogenation. The CuAl-500 catalyst showed excellent performance with 100.0% DMO conversion and 98.0% ethylene glycol (EG) selectivity, outperforming other catalysts under identical reaction conditions, and demonstrated outstanding stability for more than 200 hours. Additionally, the synergistic effect between surface Cu+ and Cu-0 sites and strengthened chemical interaction between Cu and Al species play crucial roles in DMO selective hydrogenation and suppressing the agglomeration of dispersive Cu nanoparticles during DMO hydrogenation, respectively.
Article
Chemistry, Physical
Mohamed Abbas, JiaMing Wang, Pawel Stelmachowski, Jiangang Chen, Andrzej Kotarba
Summary: Noble metal-free hydroxyapatite/graphite composite catalysts with transition metal nanoparticles were used for the hydrogenation reaction of dimethyl oxalate. CoCu/HAp/G exhibited the highest methyl glycolate selectivity of 99.3%. The increase of experimentally measured work function values was found to improve the turnover frequency and selectivity, and Cu+ ions played a role in maintaining the stability of selectivity with increasing reaction temperatures.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Hongfei Yun, Yu Zhao, Xian Kan, Guixian Li
Summary: Cu/SiO2 catalyst prepared by the ammonia-evaporation method shows high catalytic activity for the hydrogenation of dimethyl oxalate to ethylene glycol. The surface hydroxyl group of the support has significant influence on the structure and catalytic performance of the prepared Cu/ZSM-5 catalyst. The Cu/ZSM-5 catalyst prepared by pre-drying the ZSM-5 support possesses smaller particles size, higher copper dispersion, higher surface area of Cu-0 and Cu+ species, and improved catalytic activity. The catalytic activity remains stable even after 300 hours of reaction.
Article
Chemistry, Physical
Tianyou Li, Ling Lin, Chongchong Chen, Runping Ye, Long Huang, Jinxia Yang, Peng Zhang, Yeyan Qin, Jiankai Cheng, Yuangen Yao
Summary: In this study, the effect of introducing EDTA on Cu/SiO2 catalysts was systematically investigated. The introduction of an appropriate amount of EDTA not only facilitated the formation of smaller Cu nanoparticles, but also enhanced the stability of Cu species, increased the number of active sites, and strengthened the synergistic effect between Cu+ and Cu-0. The 0.08E-Cu/SiO2 catalyst exhibited the best performance and stability in the DMO hydrogenation reaction.
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
Chemistry, Physical
Runping Ye, Chong Zhang, Peng Zhang, Ling Lin, Long Huang, Yuanyuan Huang, Tianyou Li, Zhangfeng Zhou, Rongbin Zhang, Gang Feng, Yuan-Gen Yao
Summary: β-cyclodextrin (β-CD) was utilized to prepare copper-based catalysts, which showed enhanced conversion, selectivity, and lifetime for the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG).
CATALYSIS COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Shu-Qing Yang, Yin-Qing Yao, Xiao-Chao Chen, Yong Lu, Xiao-Li Zhao, Ye Liu
Summary: The study investigates the mechanism of Pd-catalyzed amino dicarbonylation of aryl halides using different ligands, with the ionic diphosphine ligand L4 showing superior catalytic performance for achieving high conversion rates and selectivity.
Article
Nanoscience & Nanotechnology
Mengchen Shen, Guofeng Zhao, Qiang Nie, Chao Meng, Weidong Sun, Jiaqi Si, Ye Liu, Yong Lu
Summary: The development of a free-standing Ni-Al2O3 ensemble derived from NiAl-layered double hydroxides (NiAl-LDHs) grown onto a Ni-foam has proven to be effective in achieving a unique combination of high activity/selectivity and enhanced heat/mass transfer. The catalyst derived from un-calcined NiAl-LDH/Ni-foam exhibits a high turnover frequency and the capability to convert a high percentage of acetone into isopropanol with almost 100% selectivity.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Qiang Nie, Guofeng Zhao, Mengchen Shen, Ye Liu, Yong Lu
Summary: A bifunctional Ni-MoOx catalyst was developed for halide-free methanol carbonylation, with its performance strongly dependent on calcination/reduction temperature. The NiMo-350-600/SiO2 catalyst showed high methanol conversion and acetyls yield, with increased acetyls formation due to the presence of Ni0 and MoOx. MoO3 and NiMoO4 favored acetyls and DME formation, while MoNi4 and MoO2 enhanced DME production.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Multidisciplinary
Xiao-Chao Chen, Yin-Qing Yao, Kai-Chun Zhao, Lei Liu, Yong Lu, Ye Liu
Summary: Ru(III)-porphyrin catalyst showed high efficiency in transforming CO2 into high value-added products, with yields of oxazolidinones reaching 71% to 91% in a three-component reaction involving aliphatic amines and dichloroethane. The cooperative activation of CO2 by aliphatic amines and dichloroethane by the catalyst contributed to the success of this transformation.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Jiaqi Si, Guofeng Zhao, Weidong Sun, Jincun Liu, Cairu Guan, Yong Yang, Xue-Rong Shi, Yong Lu
Summary: This study reports a low-temperature active and selective MnOx-Na2WO4/SiO2 catalyst for the oxidative coupling of methane (OCM). The presence of Q(2) units in the SiO2 carrier is found to significantly lower the light-off temperature of the Mn3+ <-> Mn2+ redox cycle, enhancing the catalytic activity. Additionally, Na2WO4 promotes the reaction initiation and improves the selectivity towards C2-3 products.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Kai-Chun Zhao, Lei Liu, Xiao-Chao Chen, Yin-Qing Yao, Lin Guo, Yong Lu, Xiao-Li Zhao, Ye Liu
Summary: A series of diphosphine ligands containing bis-phosphino fragments and bis-amido groups have been synthesized and their effects on the catalytic activity of Pd complexes have been investigated. Among these ligands, L5 exhibits a synergistic catalytic effect, leading to higher activity and yields in the alkoxycarbonylation reaction of alkynes with methanol.
Article
Chemistry, Physical
Guofeng Zhao, Jiayong Ni, Jiaqi Si, Weidong Sun, Yong Lu
Summary: This article reviews the recent studies on the low-temperature light-off Mn2+<-> Mn3+ redox cycle over MnOx-Na2WO4-based catalysts and highlights its positive effect on reducing the ignition temperature of OCM. In addition, three perspectives for the industrialization of OCM based on this concept are discussed.
Article
Chemistry, Physical
Xiao-Chao Chen, Tian Lan, Kai-Chun Zhao, Lin Guo, Yong Lu, Ye Liu
Summary: This study developed a new P,O-hybrid ligand and successfully synthesized a stable Rh-complex Z, which exhibited excellent catalytic activity to accelerate each individual step in the tandem hydroaminomethylation (HAM) reaction and inhibit the side-reaction of olefin-hydrogenation.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Qiang Nie, Jiaqi Si, Chao Meng, Tian Lan, Weidong Sun, Guofeng Zhao, Ye Liu, Yong Lu
Summary: The Cu/Sn-beta system enables efficient synthesis of methyl acetate with high selectivity and low methanol conversion. The catalyst facilitates the formation of bridged-adsorbed CH2O* through electron transfer and Cu(0) dehydrogenation, and further transforms it into formaldehyde through a C-C coupling reaction. Finally, formaldehyde condenses with adsorbed CH3O* on the Cu-0 site to form methyl acetate.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Xiao-Chao Chen, Tian Lan, Jian Zhu, Sibin Ying, Guang-Hui Shi, Kai -Chun Zhao, Lin Guo, Yong Lu, Ye Liu
Summary: In this study, the tripodal phosphine L1 was used to control the activity, regioselectivity, and stability of the Pd-catalyst in the synthesis of linear amides. The unique characteristics of L1, such as its steric bulkiness, switching-coordination mode, and robustness against moisture and oxygen, contributed to the high activity, good regioselectivity, and excellent stability of the Pd-catalyst.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Jiaqi Si, Guofeng Zhao, Tian Lan, Jiayong Ni, Weidong Sun, Ye Liu, Yong Lu
Summary: The study reveals that Na2WO4 plays a crucial role in reducing the trigger temperature and selectively activating the Mn7SiO12 <-> MnSiO3 redox reaction in the OCM process. It also shows that oxygen exchange between O2 and Na2WO4 only occurs in case of re-oxidizing MnWO4 formed during the reaction at high temperatures.
Article
Chemistry, Organic
Yi-Ying Zhuang, Xiao-Chao Chen, Kai-Chun Zhao, Guo-Sheng Zhang, Yu-Fen Xie, Yong Lu, Ye Liu
Summary: This work was financially supported by the National Natural Science Foundation of China (Nos. 22172052 and 21972045), and the Research Funds of Happiness Flower ECNU (2022ST2203).
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Review
Chemistry, Physical
Guofeng Zhao, Jacob A. Moulijn, Frederik Kapteijn, Frits M. Dautzenberg, Bin Xu, Yong Lu
Summary: Heterogeneous catalysis is crucial in current chemical and energy production. The use of fiber/foam-substrates with non-dipcoating methods shows great potential in addressing the limitations of traditional packed-bed reactors and improving reaction efficiency.
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING
(2023)
Article
Chemistry, Physical
Guang-Hui Shi, Xiao-Chao Chen, Tian-hong Jing, Yi-Ying Zhuang, Yong Lu, Ye Liu
Summary: The first-step hydroformylation of allyl acetate was studied for the synthesis of 1,4-butanediol via a two-step hydroformylation-hydrogenation sequence. The Xantphos-modified Rh(acac)(CO)2 catalytic system showed high efficiency, with a yield of 80% for the target product of 4-acetoxybutanal. The catalytic system exhibited excellent regioselectivity and recyclability, making it suitable for large-scale applications. Control experiments were conducted to understand the reaction pathways for the formation of the target product and related side-products.
MOLECULAR CATALYSIS
(2023)
Article
Energy & Fuels
Shuang Xue, Tian Lan, Guofeng Zhao, Qiang Nie, Chao Meng, Xinyi Xu, Yong Lu
Summary: In this study, a highly active and selective NiCx/Ni-foam catalyst is reported, which is obtained by the endogenous growth of NiC2O4 onto a Ni-foam and subsequent H2-reduction treatment. The preferred catalyst with high content of NiCx is capable of converting 63.6% or 94.3% CO at 350 degrees C or 400 degrees C with trace or < 0.8% CH4 formation for a feed gas with H2O/CO/Ar molar ratio of 4/1/9, and is stable for at least 110 h. It is experimentally and theoretically revealed that the Ni3C facilitates the dissociative activation of H2O and favors CO to form carboxylate species (favorable for CO2 formation) rather than active Ni(CO)n intermediates for CH4 formation thereby enabling the catalyst with high WGSR activity and selectivity.
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)
