Article
Chemistry, Multidisciplinary
Guanling Yang, Haobo Wang, Aizhong Jia, Jingde Li, Yanji Wang
Summary: Hierarchically porous CexZr1-xO2 materials were prepared using a simple and scalable method, and applied in the direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol. The effects of cerium sources and Zr-doping on the textural properties of the synthesized materials were investigated. The results showed that Ce0.9Zr0.1O2 had the highest catalytic activity with a DMC yield of 257.14 mmol g⁻¹, attributed to its largest specific surface area (152.1 m² g⁻¹) and highest oxygen vacancy concentration (34%).
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Engineering, Chemical
Zeyu Jiang, Shengying Zhao, Yuhao Yang, Minghui Tan, Guohui Yang, Yisheng Tan
Summary: In this study, a series of Ce-BTC MOF-derived nanorod CeO2 catalysts were prepared for the direct synthesis of DMC from CO2 and methanol. The calcination atmosphere had a great impact on the structure and catalytic properties of the obtained CeO2 catalysts. CeO2 derived from calcination under H2 atmosphere at 500 degrees C exhibited higher specific surface area, oxygen vacancy concentration, and CO2 adsorption capacity, leading to a significantly higher DMC yield compared to commercial nano CeO2 and other prepared catalysts without dehydrating agents.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Green & Sustainable Science & Technology
W. Donphai, O. Phichairatanaphong, R. Fujii, P. Li, T. Chang, M. Yabushita, Y. Nakagawa, K. Tomishige
Summary: Direct synthesis of dimethyl carbonate (DMC) is an environmentally-friendly process that utilizes CO2 as a source of useful chemicals. Various CeO2 catalysts with different properties have been employed for this reaction. In this study, CeO2 catalysts prepared via specific methods showed the highest DMC yield under certain conditions, comparable to previously reported values.
MATERIALS TODAY SUSTAINABILITY
(2023)
Article
Chemistry, Physical
Xilong Wang, Mohnnad H. Alabsi, Peng Zheng, Jinlin Mei, Adrian Ramirez, Aijun Duan, Chunming Xu, Kuo-Wei Huang
Summary: A dendritic PdCu/Ce0.3Zr0.7O2 catalyst with uniform spherical morphology was prepared and used for CO2 hydrogenation to methanol. The catalyst exhibited open dendritic pore channels and small particle sizes, which facilitated the diffusion process and increased the accessibility between active sites and reactants. The catalyst showed improved catalytic performance, with high CO2 conversion, methanol yield, PdCu-TOFMeOH, and long-term stability.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Chemistry, Physical
Zhu Fu, Ping Qi, Huimin Liu, Qijian Zhang, Yonghua Zhao, Xiaoqian Feng
Summary: Partial oxidation of dimethyl ether (DME) to hydrogen is an efficient route for hydrogen production for application in SOFC. However, the production of a large amount of CO2 as a byproduct has been a significant obstacle. In this study, cerium-zirconium solid solution was used as a catalyst to investigate the effect of its oxidative properties on CO2 production during the partial oxidation of DME. The results show that a catalyst with more adsorbed oxygen exhibits higher DME conversion and CO2 yield due to the overoxidation of CO.
Article
Chemistry, Physical
Shiyu Xu, Yunxia Cao, Zhiming Liu
Summary: CexZr1-xO2 catalysts were prepared by the sol-gel method and used for the direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol. Ce0.8Zr02O2 catalyst exhibited the highest catalytic activity, which may be attributed to its highest concentration of oxygen vacancy sites.
CATALYSIS COMMUNICATIONS
(2022)
Article
Energy & Fuels
Zhen-Hong He, Yong-Chang Sun, Yuan-Yuan Wei, Kuan Wang, Weitao Wang, Zhuo Chen, Zhong-Yu Wang, Yue Tian, Zhao-Tie Liu
Summary: This study developed a catalyst of CeO2 nanoparticles loaded on Co3O4 nanosheets that efficiently catalyze the reaction between methanol and CO2 to synthesize dimethyl carbonate (DMC). The catalyst exhibited high activity and yield of DMC by enhancing oxygen vacancies and CO2 adsorption while reducing methanol adsorption. The catalyst can simultaneously activate CO2 and methanol and the reaction follows a Langmuir-Hinshelwood mechanism.
Review
Biochemistry & Molecular Biology
Yifei Zhang, Muhammad Shoaib Khalid, Meng Wang, Gao Li
Summary: This review paper discusses the green production methods of DMC using Zr/Ce/Cu-based nanocomposites as catalysts, including the relationship between the structure and activity of catalysts, catalytic mechanisms, molecular activation and active sites identification of catalysts.
Article
Chemistry, Physical
Linmeng Huo, Tian Wang, Keng Xuan, Lei Li, Yanfeng Pu, Chenxin Li, Congzhen Qiao, Hao Yang, Yan Bai
Summary: The distance between Zr4+ and Zr4+/O2- sites in Zr-based catalysts has a significant impact on the adsorption and activation of CO2 and methanol. The Zr/SBA-15 catalyst with adjacent sites showed good catalytic activity, while no DMC was detected over the Zr-SBA-15 catalyst.
Article
Chemistry, Multidisciplinary
Mingjuan Sun, Fengjiao Li, Yanhui Cui, Xiaolin Zhao, Haiwei Chen, Shuting Liang
Summary: Dimethyl carbonate (DMC) has been synthesized efficiently and mild by the electrochemical method using urea and methanol as starting materials. The highest DMC yield of 50.4% with 100% selectivity was achieved under optimized conditions. This method also successfully synthesized other important organic carbonates.
REACTION CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Wei Xu, Zhihao Xu, Wenxuan Yao, Lihua Hu, Keqiang Ding, Gongde Wu, Guomin Xiao, Lijing Gao
Summary: UiO-66@CeO2 composites were prepared by loading CeO2 nanoparticles on the surface of UiO-66 using precipitation method, and the effect of CeO2 loading on the catalytic direct reaction of CO2 and methanol into dimethyl carbonate (DMC) was investigated. The results showed that UiO-66 framework structure benefited the high dispersion of CeO2, and the loading of CeO2 provided more oxygen vacancies, promoting the capture and absorb of CO2 and thus promoting the reaction synergistically. UiO-66@CeO2-60 exhibited the highest DMC formation rate of 2.84 mmol.g(-1).h(-1) (yield: 2.27%) within 4 h of reaction time under the optimum conditions, and the catalyst also showed favorable reusability maintaining similar to 90% of catalytic efficiency with 4 reuse cycles compared to the fresh ones.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Multidisciplinary
Keng Xuan, Shikun Chen, Yanfeng Pu, Yaoping Guo, Yadan Guo, Yun Li, Chenxi Pu, Ning Zhao, Fukui Xiao
Summary: In this study, a HPW@MOF-808 catalyst was successfully prepared and demonstrated to have high activity and good stability in the direct synthesis of DMC. The encapsulation of HPW in the micropores of MOF-808 increased its interaction with Zr-6 nodes, resulting in the generation of more acid sites and promoting the formation of methyl cations (rate-determine step in DMC synthesis). Additionally, the encapsulated HPW inhibited leaching during the reaction, leading to better reusability.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Chemistry, Multidisciplinary
Fei Chen, Wensheng Wei, Yunsheng Gao, Yuxin Wang, Zizhen Yan, Zhanguo Zhang, Haiming Yu, Guangwen Xu, Lei Shi
Summary: Ionic liquid [Emim]IM with high thermal stability and strong basicity was synthesized and used as a catalyst for the direct synthesis of dimethyl carbonate (DMC). The [Emim]IM catalyst exhibited good stability and catalytic activity.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Engineering, Chemical
Saheli Biswas, Chandan Kundu, Aniruddha P. Kulkarni, Shyam Kattel, Sarbjit Giddey, Sankar Bhattacharya
Summary: Fe-impregnated CexZr1-xO2 supports show higher CO2 conversion and CH4 yield compared to Fe-impregnated ZrO2, especially at higher temperatures, indicating potential for improved catalytic performance in CO2 methanation reactions.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Bo Jia, Xiaoyu Sun, Ming Chen, Jian Jian, Kuiyi You, He'an Luo, Yangqiang Huang, Xiao Luo, Bo Jin, Nailiang Wang, Zhiwu Liang
Summary: This paper evaluates an optimal composite metal oxide ZnAl-LDO catalyst, prepared from Zn/Al layered double hydroxides (ZnAl-LDHs), for the synthesis of dimethyl carbonate (DMC) through methyl carbamate (MC) alcoholysis. The catalyst achieved high selectivity for DMC production under optimal conditions and its catalytic performance was investigated through structural characteristics, kinetic modeling, and thermodynamic calculations.
REACTION CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Physical
Long-Yao Li, Zhong-Yu Wang, Shao-Yan Yang, Jian-Gang Chen, Zhen-Hong He, Kuan Wang, Qun-Xing Luo, Zhong-Wen Liu, Zhao-Tie Liu
Summary: In this study, Fe-doped silicalite-1 zeolite was used as a matrix to implant GaN nanocrystallites. The incorporation of isolated framework Fe atoms resulted in the generation of more interior silanols and silanol nests, leading to the formation of highly dispersed GaN nanocrystallites embedded in the Fe-silicalite-1 matrix. The particle size distribution of GaN could be adjusted by regulating the molar ratio of Si/Fe.
Article
Chemistry, Multidisciplinary
Weitao Wang, Liqiong Ma, Xulu Jiang, Huan Wang, Zhen-Hong He, Kuan Wang, Yang Yang, Zhao-Tie Liu
Summary: This study developed a new approach for the cyanide-free synthesis of organic nitriles through highly direct oxidative cyanation of alcohols. By using a CoOx/MnO2 catalyst under aqueous ammonia conditions, benzyl alcohol was successfully converted to benzonitrile with high yield and selectivity. Kinetic studies revealed that the oxidation of benzyl alcohol was the rate-determining step in the consecutive reactions. The catalytic system also demonstrated its applicability to various types of alcohol substrates, showcasing a sustainable synthesis strategy.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Nanoscience & Nanotechnology
Han-Xiao Wang, Xin-Yu Zhao, Jin-Qiang Jiang, Zhao-Tie Liu, Zhong-Wen Liu, Guo Li
Summary: Thermal-responsive hydrogel actuators with programmable external shapes and internal actuating trajectories have been developed in this study, offering a wide temperature range of volume phase transition. The combination of photo-responsive shape memory property and gradient crosslinking enables more flexible and intricate shape-changing behaviors, with potential applications in lifting objects with specific shapes. The proposed strategy can be extended to other types of actuating hydrogels for more advanced actuating behaviors.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Inorganic & Nuclear
Junlei Wang, Kuan Wang, Zhen-Hong He, Tong Sun, Run-Jing You, Jian-Gang Chen, Weitao Wang, Yang Yang, Zhao-Tie Liu
Summary: Bi2WO6 with double active sites of tunable metallic Bi and oxygen vacancies (OV-Bi/Bi2WO6) was prepared by solvothermal treatment and used as an efficient photocatalyst for the partial oxidation of cyclohexane (CHA) to cyclohexanone (CHA-one) in air. The Bi : Bi2WO6 ratio in OV-Bi/Bi2WO6 could be tailored by controlling the solvothermal temperature, and the synergistic effect between DMF and EG increased the reduction of MDF/EG and promoted the production of Bi. OV-Bi/Bi2WO6 showed significantly enhanced photocatalytic activity attributed to its specific surface area, photo-absorption, oxygen vacancies, and efficient electron-hole separation.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Yang Yang, Qian-Nan Yang, Yi-Bin Yang, Peng-Fei Guo, Wan-Xin Feng, Yan Jia, Kuan Wang, Wei-Tao Wang, Zhen-Hong He, Zhao-Tie Liu
Summary: Designing a highly active single atom catalyst, particularly noble-metal atoms in two-dimensional LDH nanostructures, is essential for speeding up the slow oxygen evolution reaction (OER). By reducing a solution, Ru single atoms (SAs) are fixed on NiFe LDH to form SARu/NiFe LDH. The activity evaluation shows that SARu/NiFe LDH exhibits higher activity and Faradaic efficiency compared to pure NiFe LDH.
Article
Nanoscience & Nanotechnology
Ling Hu, Jinqiang Jiang, Zhao-Tie Liu, Zhong-Wen Liu, Guo Li
Summary: A simplified treatment process is reported to convert 2D poly(ethylene oxide)/sodium alginate/tannic acid thin films into 3D-shaped moisture- and NIR light-responsive actuators. Wetting the film surface releases residual stress in a gradient manner, driving the wetted regions to bend bidirectionally. A gradient cross-linking network formed by Fe3+ ions and sodium alginate chains stabilizes the resulting 3D shape and provides moisture-responsive morphing behaviors. Fe3+ ions also enable the film to respond to NIR light by self-assembling with tannic acid molecules. Films with versatile 3D shapes and deformation modes can be conveniently fabricated using this one-step treatment process.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Xiangxi Cui, Min Dang, Jinqiang Jiang, Zhao-Tie Liu, Zhong-Wen Liu, Guo Li
Summary: In this study, a photoresponsive elastic composite is developed, which can be programmed and transformed into different shapes through UV light irradiation and stretching. The composite exhibits adjustable shape and strain-sensitive conductivity, which opens up possibilities for designable soft electronics.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Weitao Wang, Liqiong Ma, Huan Wang, Xulu Jiang, Zhen-Hong He, Kuan Wang, Yang Yang, Lu Li, Zhao-Tie Liu
Summary: In this study, a Se,P,N-tridoped carbon nanomaterial (Se,P,N/CN-900) was successfully prepared and used as a metal-free catalyst for the direct ammoxidation of alcohols to nitriles with aqueous ammonia and molecular oxygen. The tridoped carbon catalyst exhibited highly efficient catalytic performance and good stability, enabling the conversion of various (hetero)aromatic alcohols to corresponding nitriles with high yields. To the best of our knowledge, this is the first work to achieve ammoxidation of alcohols to nitriles with a high efficiency over multidoped carbon materials.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Yang Yang, Qian-Nan Yang, Yi-Bin Yang, Peng-Fei Guo, Wan-Xin Feng, Yan Jia, Kuan Wang, Wei-Tao Wang, Zhen-Hong He, Zhao-Tie Liu
Summary: Designing and synthesizing highly active single atom catalysts, especially monodispersed noble-metal atoms fixed in two-dimensional layered double hydroxide (LDH) nanostructures, is crucial for accelerating the slow oxygen evolution reaction (OER). In this study, Ru single atoms (SAs) were stabilized on NiFe LDH (SARu/NiFe LDH) via an oxygen-coordinated bond after a facile solution reduction procedure. The SARu/NiFe LDH exhibits higher activity than pure NiFe LDH in basic media, with 99.3% Faradaic efficiency based on rotating ring-disk electrode measurement. This study provides a general avenue for developing efficiently monoatomic and even multiatomic catalysts in the future.
Review
Chemistry, Physical
Yukun Ruan, Zhen-Hong He, Zhao-Tie Liu, Weitao Wang, Leiduan Hao, Liang Xu, Alex W. Robertson, Zhenyu Sun
Summary: This review summarizes the important progress in the electroreduction of N2 to NH3 using state-of-the-art two-dimensional (2D) electrocatalysts. Several reaction mechanisms of nitrogen reduction reaction (NRR) are explained, and recent experimental progress regarding these unique 2D NRR electrocatalysts is reported. Furthermore, concepts proposed from high-throughput computations and machine learning are described. By understanding the N2 conversion to NH3 process on 2D electrocatalysts, novel 2D materials that could potentially serve as viable NRR electrocatalysts are presented. The future perspectives and challenges of N2 electrolysis using 2D materials are also discussed.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Zhen-Hong He, Cui-Cui Li, Shao-Yan Yang, Jiajie Liu, Hui-Hui Cao, Kuan Wang, Weitao Wang, Yang Yang, Zhao-Tie Liu
Summary: In this study, a series of easily prepared CuOx catalysts were developed and applied in CO2 electrocatalytic reduction to synthesize ethylene; the introduction of neodymium stabilizes the catalyst and enhances CO2 adsorption; coupling *CO with ethylene further improves the Faradaic efficiency of ethylene.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Physical
Yukun Ruan, Zhen-Hong He, Zhao-Tie Liu, Weitao Wang, Leiduan Hao, Liang Xu, Alex W. Robertson, Zhenyu Sun
Summary: “This review summarizes the significant progress in electroreduction of N2 to NH3 using state-of-the-art two-dimensional (2D) electrocatalysts. Several reaction mechanisms of NRR are explained and recent experimental progress on these unique 2D NRR electrocatalysts is reported. Additionally, concepts proposed from high-throughput computations and machine learning are discussed. Novel 2D materials that have the potential to serve as viable NRR electrocatalysts are presented based on a detailed understanding of the N2 conversion process on 2D electrocatalysts. Future perspectives and challenges of N2 electrolysis using 2D materials are also addressed.”
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Xulu Jiang, Weitao Wang, Huan Wang, Zhen-Hong He, Yang Yang, Kuan Wang, Zhao-Tie Liu, Buxing Han
Summary: A Z-scheme heterojunction photocatalyst of ZnO/C3N4 was designed and prepared for the selective oxidation of benzyl alcohol to benzaldehyde under solvent-free conditions. The results showed that benzyl alcohol could be exclusively oxidized to benzaldehyde with high yield and formation rate at room temperature. The photocatalytic activity and selectivity of this system were better than those of noble and non-noble metal-based photocatalyses.
Article
Chemistry, Multidisciplinary
Zhen-Hong He, Bao-Ting Wu, Zhong-Yu Wang, Shao-Yan Yang, Kuan Wang, Jiao-Jiao Shi, Meng-Xin He, Weitao Wang, Zhao-Tie Liu
Summary: In this study, CO2-ODHP reaction was conducted for the first time at relatively low temperature and under photothermal conditions using BiOX nanocatalysts. Among them, the BiOI nanosheet catalyst exhibited high propylene formation activity and CO2 reduction activity. The lattice oxygen species on the catalyst catalyzed propane dehydrogenation to propylene, and simultaneously formed oxygen vacancies for CO2 reduction.
Article
Chemistry, Multidisciplinary
Huan Wang, Weitao Wang, Xulu Jiang, Zhen-Hong He, Kuan Wang, Yang Yang, Zhao-Tie Liu, Buxing Han
Summary: In this study, a fast and self-propagated carbonization (SPC) method was proposed for the preparation of phosphorus-doped carbon (PDC) and hybrid materials. PdZr/PDC prepared by the SPC method exhibited excellent catalytic performance in the partial oxidation of benzyl alcohol to benzaldehyde and the partial hydrogenation of phenol to cyclohexanone. The method is simple, clean, and suitable for large-scale material preparation.