Article
Energy & Fuels
Weili Jiang, Jicong Li, Mengying Wu, Limei He, Guanglin Zhou, Zhongrong Wang
Summary: Three kinds of porous organic polymers (POPs) containing N or P atoms were prepared and used as supports for Rh catalysts. The structures and compositions of these polymers were fully characterized. The Rh-N-POP showed a larger BET surface area and pore volume due to the bulk extrusion of triphenylphosphine (TPP) unit. The hydroformylation activity was promoted by the presence of free ligands in Rh-N-POP, but isomerization was greatly promoted by the TPP structure.
Review
Chemistry, Multidisciplinary
Boyang Liu, Yu Wang, Ning Huang, Xiaocheng Lan, Zhenhua Xie, Jingguang G. Chen, Tiefeng Wang
Summary: This review summarizes the developments of catalysts for heterogeneous hydroformylation in the last decade and proposes potential modification methods for future improvements. The hydroformylation properties of different reactants are compared in order to emphasize the unique challenges faced by various olefins. The catalytic properties can be tuned through electronic effects, steric hindrance, and reaction condition optimization.
Article
Biochemistry & Molecular Biology
Jeremy Ternel, Adrien Lopes, Mathieu Sauthier, Clothilde Buffe, Vincent Wiatz, Herve Bricout, Sebastien Tilloy, Eric Monflier
Summary: The synthesis of bis-primary alcohols from isosorbide diallyl ether was achieved with a rhodium/amine catalytic system, resulting in a 79% yield.
Article
Chemistry, Multidisciplinary
Chryslain Becquet, Francois Berche, Herve Bricout, Eric Monflier, Sebastien Tilloy
Summary: A catalytic system based on Rh(acac)(CO)(2) and a trialkylamine was used to synthesize polyhydroxylated derivatives from castor oil and ethyl ricinoleate, showing high yields and applicability in bio-based polyesters and polyurethanes. By optimizing the reaction conditions, alcohols were obtained at yields of 74% and 80% for castor oil and ethyl ricinoleate, respectively.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Review
Chemistry, Physical
Shangkun Li, Rizwan Ahmed, Yanhui Yi, Annemie Bogaerts
Summary: This review summarizes the latest advances in heterogeneous catalysis and plasma catalysis for direct oxidation of methane to methanol (DOMTM), aiming to point out the differences between the two and provide insights into their reaction mechanisms, as well as implications for future development of highly selective catalysts for DOMTM.
Article
Chemistry, Multidisciplinary
Kang Zhao, Hongli Wang, Xinzhi Wang, Xinjiang Cui, Feng Shi
Summary: A novel porous organic polymer catalyst was developed for the heterogeneous hydroaminomethylation of alkenes, resulting in improved regioselectivity.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Organic
D. N. Gorbunov, M. V. Nenasheva, R. P. Matsukevich, M. V. Terenina, Yu. S. Kardasheva, E. A. Karakhanov
Summary: A phosphine-containing porous polymer (TPDB) and its rhodium-based catalyst have been successfully synthesized, showing good catalytic activity in model reactions. Experimental results demonstrate that the catalyst can be reused multiple times with consistent activity.
PETROLEUM CHEMISTRY
(2021)
Review
Chemistry, Physical
Kang Zhao, Xinzhi Wang, Dongcheng He, Hongli Wang, Bo Qian, Feng Shi
Summary: This review summarizes the research progress on catalytic materials that combine homo- and heterogeneous catalysis in hydroformylation, including their synthesis, material characteristics, and applications. It also provides prospects for their future development.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Weixiang Shang, Bin Qin, Mingyang Gao, Xuetao Qin, Yuchao Chai, Guangjun Wu, Naijia Guan, Ding Ma, Landong Li
Summary: In this study, we report the construction of a zeolite-encaged rhodium catalyst for efficient hydroformylation. The catalyst exhibits high catalytic activity, perfect chemoselectivity, and recyclability, making it a promising solution for potential applications. The detailed mechanism of alkene hydroformylation can be interpreted through the well-defined structure of the catalyst.
Article
Nanoscience & Nanotechnology
Baiyin Wei, Xiaofang Liu, Kaimin Hua, Yuchao Deng, Hui Wang, Yuhan Sun
Summary: Effective control of the microenvironment of active sites is crucial for improving the selectivity of products in heterogeneous homogeneous processes. The development of a high-performance Rh-based atomically dispersed catalyst demonstrates that rational design of the local microenvironment of active metals is important to optimize catalytic performance.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Inorganic & Nuclear
Rohit Kumar, Samir H. Chikkali
Summary: Metal-catalyzed hydroformylation of alkenes is widely employed for the synthesis of aldehydes, with rhodium being the most commonly used metal catalyst. However, due to rhodium's rarity, high cost, and depletion, finding alternative catalysts is of great interest. This review summarizes the recent advancements in hydroformylation using metals other than rhodium, highlighting cobalt as the only metal that poses a significant challenge to rhodium's dominance.
JOURNAL OF ORGANOMETALLIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Seungyeon Lee, Abhirup Patra, Phillip Christopher, Dionisios G. Vlachos, Stavros Caratzoulas
Summary: Atomically dispersed late transition-metal catalysts show high activity and selectivity on supports, attributed to unique electronic properties and promoters modifying the local environment. Density functional theory calculations and microkinetic modeling reveal extensive mechanistic knowledge about the cooperativity of Rh-ReOx pairs.
Article
Chemistry, Physical
Partha Samanta, Albert Sole-Daura, Remy Rajapaksha, Florian M. Wisser, Frederic Meunier, Yves Schuurman, Capucine Sassoye, Caroline Mellot-Draznieks, Jerome Canivet
Summary: Molecularly defined organometallic rhodium phosphine complexes were efficiently immobilized within a MOF structure, maintaining their molecular nature and catalytic behavior. The resulting MOF-heterogenized catalysts showed high activity in ethylene hydroformylation and successfully catalyzed the hydroformylation of longer and bulkier alkenes. The study also provided insights into the structure, evolution, and mechanisms of the active species within the MOF under catalytic conditions.
Article
Chemistry, Physical
Partha Samanta, Albert Sole-Daura, Remy Rajapaksha, Florian M. Wisser, Frederic Meunier, Yves Schuurman, Capucine Sassoye, Caroline Mellot-Draznieks, Jerome Canivet
Summary: Molecularly defined organometallic rhodium phosphine complexes were immobilized within a MOF structure without losing their molecular nature and catalytic behavior. These MOF-based catalysts showed high activity for ethylene hydroformylation and successfully catalyzed the hydroformylation of longer and bulkier alkenes. The combination of experimental and computational methods allowed for a better understanding of the active species and molecular mechanisms involved in the catalytic reactions. The use of MOF-808 as a solid ligand offers advantages such as molecular-scale understanding, site isolation, and recycling ability.
Article
Chemistry, Organic
Tim Meyer, Robert Konrath, Paul C. J. Kamer, Xiao-Feng Wu
Summary: Formaldehyde is an important bulk chemical, and the challenge of producing valuable ethylene glycol directly from it has been a difficult one. Existing systems have low efficiency in generating ethylene glycol, but this new Rh catalyst system allows for efficient synthesis under milder conditions.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Engineering, Biomedical
Xueying Huang, Jie Zeng, Yi Wang
Summary: This study found that zein, a plant protein, can be used to create a surface that mimics the extracellular matrix, promoting the attachment and proliferation of stem cells. Zein is more effective than gelatin and silk fibroin in promoting stem cell growth. The stem cells prefer to grow in grooves that are similar in size to themselves.
JOURNAL OF BIOMEDICAL MATERIALS RESEARCH PART B-APPLIED BIOMATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Dong Cao, Zhirong Zhang, Yahui Cui, Runhao Zhang, Lipeng Zhang, Jie Zeng, Daojian Cheng
Summary: In this study, highly active catalysts consisting of high-density Pt and Ir single atoms anchored on Co(OH)(2) were constructed for green hydrogen production. The catalysts exhibited excellent catalytic activity and efficiency in alkaline water electrolysis, demonstrating great potential for practical applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Zhirong Zhang, Peiyu Ma, Lei Luo, Xilan Ding, Shiming Zhou, Jie Zeng
Summary: Regulating the spin state of active centers in transition metal oxides is of great significance in energy conversion processes. It directly modulates the metal-ligand bond strength and intermediate adsorption behavior. This review clarifies the importance of regulating the spin state and discusses characterization technologies and strategies to regulate the spin state. Lastly, future research directions in this field are proposed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Yongxiang Liang, Jiankang Zhao, Yu Yang, Sung-Fu Hung, Jun Li, Shuzhen Zhang, Yong Zhao, An Zhang, Cheng Wang, Dominique Appadoo, Lei Zhang, Zhigang Geng, Fengwang Li, Jie Zeng
Summary: The authors report a coordination polymer catalyst with isolated neighboring copper sites that can efficiently reduce CO2 to C2H4 with high selectivity and stability under electrochemical conditions. This finding is significant for achieving net-zero carbon emissions through electrochemical CO2 reduction with renewable electricity.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Jiawei Li, Hongliang Zeng, Xue Dong, Yimin Ding, Sunpei Hu, Runhao Zhang, Yizhou Dai, Peixin Cui, Zhou Xiao, Donghao Zhao, Liujiang Zhou, Tingting Zheng, Jianping Xiao, Jie Zeng, Chuan Xia
Summary: The researchers achieved CO2 reduction at high current density with a Faradaic efficiency over 95% by tuning the CO selectivity of copper through alloying, using an antimony-copper single-atom alloy catalyst.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Applied
Peiyu Ma, Chen Feng, Huihuang Chen, Jiawei Xue, Xinlong Ma, Heng Cao, Dongdi Wang, Ming Zuo, Ruyang Wang, Xilan Ding, Shiming Zhou, Zhirong Zhang, Jie Zeng, Jun Bao
Summary: To improve the efficiency of water electrolyzers, active electrocatalysts are needed for the oxygen evolution process. This study combines in-situ anionic leaching and atomic deposition to create single-atom catalysts with self-optimized structures. The results demonstrate the effectiveness of this in-situ optimization process in enhancing the performance of the catalyst.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Chuanhao Wang, Junjie Du, Lin Zeng, Zhongling Li, Yizhou Dai, Xu Li, Zijun Peng, Wenlong Wu, Hongliang Li, Jie Zeng
Summary: The authors develop a universal strategy to synthesize extra-heavy olefins through the sustained release of hydrogen and selective extraction of olefins. They achieve the selective production of C(12+)(=) from CO and water using Pt/Mo2N and Ru particles as catalysts in polyethylene glycol (PEG). PEG acts as a selective extraction agent to hinder hydrogenation of olefins. Under optimal conditions, the yield ratio of CO2 to hydrocarbons reaches the theoretical minimum, and the C(12+)(=) yield reaches its maximum with a selectivity of 40.4%.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Weiqing Xue, Xinyan Liu, Chunxiao Liu, Xinyan Zhang, Jiawei Li, Zhengwu Yang, Peixin Cui, Hong-Jie Peng, Qiu Jiang, Hongliang Li, Pengping Xu, Tingting Zheng, Chuan Xia, Jie Zeng
Summary: The removal of acetylene impurities is important yet challenging to the ethylene downstream industry. Renewable electricity-based electrocatalytic semihydrogenation of acetylene over Cu-based catalysts is an attractive alternative to thermocatalytic processes. However, active Cu electrocatalysts often face competition from side reactions. Here, an undercoordinated Cu nanodots catalyst is reported with excellent C2H2-to-C2H4 catalytic activity.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Haibin Yin, Zhengtian Pu, Jiawei Xue, Peiyu Ma, Bo Wu, Mei Han, Hongfei Lin, Zhengtang Luo, Jie Zeng, Xinlong Ma, Hongliang Li
Summary: TiO2 nanorods with abundant oxygen vacancies enable the mild oxidation of methane by H2O2 into formaldehyde without light irradiation. The activity of TiO2 nanorods increases with the concentration of oxygen vacancies. The reaction intermediates and reaction scheme were identified based on catalytic and spectroscopic data.
Article
Chemistry, Physical
Yinyin Wang, Jiankang Zhao, Cong Cao, Jie Ding, Ruyang Wang, Jie Zeng, Jun Bao, Bin Liu
Summary: Selective electrochemical reduction of CO to acetate can be achieved on an amino functionalized Cu surface. The Cu@NH2 catalyst shows significant catalytic performance with a CO-to-acetate Faradaic efficiency of 51.5% and an acetate partial current density of around 150 mA cm-2 at -0.75 V versus RHE. The amino groups on the Cu surface help maintain the low valence state of Cu and the H delta+ in the amino groups stabilize the oxygen-containing intermediates, promoting the formation of acetate through *CO-*CHO coupling.
Article
Nanoscience & Nanotechnology
Junjie Du, Lin Zeng, Tao Yan, Chuanhao Wang, Menglin Wang, Lei Luo, Wenlong Wu, Zijun Peng, Hongliang Li, Jie Zeng
Summary: Ru nanoparticles on HZSM-5 catalyze solvent- and hydrogen-free upcycling of high-density polyethylene into separable linear (C-1 to C-6) and cyclic (C-7 to C-15) hydrocarbons. Plastic pollution, worsened by the COVID-19 pandemic, requires a sustainable and economically viable recycling method that avoids consumable materials. This study demonstrates the catalytic conversion of high-density polyethylene using Ru nanoparticles on HZSM-5, resulting in a separable distribution of linear and cyclic hydrocarbons.
NATURE NANOTECHNOLOGY
(2023)
Review
Chemistry, Physical
Jinli Yu, Juan Xiao, Yangbo Ma, Jingwen Zhou, Pengyi Lu, Kun Wang, Yan Yan, Jie Zeng, Yi Wang, Shuqin Song, Zhanxi Fan
Summary: In this article, we review the recent advances in electrochemical CO2RR in acidic media. We discuss the impact of acidic conditions on the carbon efficiency of CO2RR, strategies for modulating performance, and catalyst development. We also highlight the research challenges and provide our perspectives on CO2RR in acidic media.
Article
Chemistry, Physical
Lei Luo, Zekun Zeng, Tao Zhou, Jun Luo, Xiaoheng Chen, Xu Li, Han Yan, Jie Zeng
Summary: In this study, PtFe/SiO2 catalyst was successfully prepared and showed excellent performance for non-oxidative propane dehydrogenation (PDH), efficiently producing propylene. The introduction of Fe component in the catalyst facilitated the high dispersion of Pt, preventing its agglomeration. Electron-rich Pt sites were formed in PtFe/SiO2, enhancing both propylene formation rate and mean lifetime. This work provides a pathway for developing robust Pt-based PDH catalysts through alloying with earth-abundant metals.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Yinyin Wang, Jiankang Zhao, Cong Cao, Jie Ding, Ruyang Wang, Jie Zeng, Jun Bao, Bin Liu
Summary: Electrosynthesis of valuable chemicals from CO2 or CO offers a promising approach to store renewable electricity and reduce carbon emission. In this study, amino functionalized Cu surface (Cu@NH2) derived from in situ electroreduction of copper ammonia chloride complexes exhibits significant catalytic performance for CO reduction to acetate. The amino groups on the Cu surface play a crucial role in maintaining the low valence state of Cu and stabilizing the oxygen-containing intermediates, thus promoting the coupling reaction between *CO and *CHO to form acetate.