Article
Chemistry, Inorganic & Nuclear
Zhi-Qiang Wang, Cheng-Hua Deng, Xiao Liu, Wen-Min Wang
Summary: In this study, a green-synthesis produced aluminum-based metal-organic framework (Al-MOF) material CAU-10pydc was used as a catalyst for CO2 formylation reaction. The results showed that CAU-10pydc could effectively catalyze the reaction of CO2 and N-methylaniline to N-methyl-N-phenylformamide under mild conditions. CAU-10pydc maintained its efficient catalytic performance after cyclic catalysis and exhibited stability. The universality of this catalyst was demonstrated through reactions with nine substrates. This work represents the first example of a highly effective Al-MOF catalyzing CO2 formylation reaction under green conditions.
DALTON TRANSACTIONS
(2023)
Article
Multidisciplinary Sciences
Rong-Hua Wang, Wei-Wei Xu, Hongli Wu, Yue Li, Jiang-Fei Li, Tao Zhang, Genping Huang, Mengchun Ye
Summary: In this study, we report a new phosphine oxide-ligated Ni-Al bimetallic catalyst that can efficiently activate secondary benzylic C-H bonds via 4-membered nickelacycles, leading to the synthesis of high-yield α,β-unsaturated γ-lactams.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Shuang-Shuang Ma, Rui Sun, Zi-Heng Zhang, Peng-Xin Guan, Jin-Qing Lin, Chun-Shan Li, Bao-Hua Xu
Summary: A novel half-sandwich phosphinesulfonate cobaltic complex was prepared and used for the chemoselective N,N-dimethylation of nitroaromatics. The catalytic activity could be modulated by using specific hydrosilanes.
Article
Chemistry, Multidisciplinary
Matthias Elfinger, Timon Schoenauer, Sabrina L. J. Thomae, Robert Staeglich, Markus Drechsler, Mirijam Zobel, Juergen Senker, Rhett Kempe
Summary: The 3D metal catalyst developed here utilizes hydrogen as the reducing agent and easily handled ammonia dissolved in water as the nitrogen source for the synthesis of primary amines. The catalyst operates under mild conditions and outperforms commercially available noble metal catalysts. The key to its high activity is the unique support material it uses.
Letter
Chemistry, Organic
Shaocheng Li, Thayalan Rajeshkumar, Jincheng Liu, Laurent Maron, Xigeng Zhou
Summary: Here, we describe a redox-neutral rare earth catalyst that enables the first catalytic decarbonylation and decarbonylative hydroamination of formamides without using additives. The protocol exhibits complete N-aryl/alkenyl formamide-selectivity, thus offering a diverse range of possibilities for N-formylation and N-deformylation methods, and opening up new prospects for waste reduction and control of selectivity in amine transformation events.
Article
Chemistry, Organic
Yipeng Zhou, Hongwei Zhou, Jianfeng Xu
Summary: A highly selective [3+2] cycloaddition reaction was achieved using a chiral catalyst, resulting in the synthesis of enantioenriched bicyclic pyrazolidinones.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Organic
Lvyin Zheng, Liuhuan Cai, Weijie Mei, Gongping Liu, Ling Deng, Xiaoying Zou, Xiaoya Zhuo, Yumei Zhong, Wei Guo
Summary: In this study, an efficient copper-catalyzed aerobic oxidative cross-dehydrogenative coupling reaction was developed for the synthesis of multisubstituted phosphorylhydrazides. The reaction proceeded under mild conditions without the need for any external oxidants and bases. The selected compounds exhibited potential inhibitory activity against tumor cells, making them suitable for the screening of anticancer agents.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Organic
Priyanka Adhikari, Dipanjan Bhattacharyya, Sekhar Nandi, Pavan K. Kancharla, Animesh Das
Summary: The study demonstrates that a boronic acid-catalyzed one-pot tandem reaction can achieve the synthesis of N-alkyl tetrahydroquinolines from quinolines, aldehydes, and Hantzsch ester in a step-economical manner under mild reaction conditions. The mechanistic study shows the unique behavior of organoboron catalysts acting as both Lewis acids and hydrogen-bond donors.
Article
Chemistry, Multidisciplinary
Peiyuan Yao, James R. Marshall, Zefei Xu, Jesmine Lim, Simon J. Charnock, Dunming Zhu, Nicholas J. Turner
Summary: In this study, a new stereoselective biocatalytic synthesis method for N-substituted alpha-amino esters was reported, utilizing diverse metagenomic imine reductases. Both enantiomers of the target products were synthesized with high conversion and excellent enantioselectivity under mild reaction conditions. Furthermore, over 20 different preparative scale transformations were performed, demonstrating the scalability of this system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Applied
Guohui Zhang, Qianqian Liang, Wei Yang, Shaohua Jiang, Zhiping Wang, Chunyan Zhang, Guoying Zhang
Summary: Reductive homocoupling transformations mediated by bases and TMSCN have been utilized for the synthesis of 1,2-disubstituted ethanones. This protocol offers a method for the synthesis of functionalized ethanones from aldehydes without the need for transition metals, all in a single reaction vessel.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Wenyuan Huang, Qingqing Mei, Shaojun Xu, Bing An, Meng He, Jiangnan Li, Yinlin Chen, Xue Han, Tian Luo, Lixia Guo, Joseph Hurd, Daniel Lee, Evan Tillotson, Sarah Haigh, Alex Walton, Sarah Day, Louise Natrajan, Martin Schroeder, Sihai Yang
Summary: This study reports the direct synthesis of N-formamides by coupling reductive amination of carbonyl compounds and CO2 fixation. A ruthenium catalyst supported by a metal-organic framework was used to achieve highly selective production of N-formamides. The presence of host-guest binding interactions between the catalyst and adsorbed substrates facilitated the activation of substrates and promoted selectivity.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Applied
Fan Yang, Yuta Saiki, Koichi Nakaoka, Tadashi Ema
Summary: This study reported the solvent-free N-formylation reaction catalyzed by Cu(OAc)(2), which used CO2 and phenylsilane to react with 2-(methylamino)pyridine and produced N-methyl-N-(2-pyridyl)formamide. The improved solubility of copper ion and enhanced nucleophilicity of acetate ion played positive roles in the activation of phenylsilane.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Chemistry, Organic
Ryukichi Takagi, Duyen Thi Duong
Summary: This study used density functional theory calculations to investigate the mechanism of enantioselective intramolecular hydroamination catalyzed by chiral binaphthol N-triflylphosphoramide (NPTA). It reveals the details of the hydrogen bonding mode between NPTA and the substrate, emphasizing the importance of the dual hydrogen binding properties of the thiourea moiety for the reactivity and stereoselectivity of the hydroamination.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2021)
Article
Chemistry, Organic
Jiayong Zhang, Zhengjie He
Summary: A Lewis base-catalyzed intramolecular vinylogous aldol reaction has been developed for the synthesis of 3-hydroxy-2,3-disubstituted dihydrobenzofurans and indolines with high yields, excellent chemoselectivity, and diastereoselectivity. The resulting products can be further utilized for the synthesis of 2-alkenyl benzofurans and indoles through acid-promoted dehydration.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Zhiqiang Guo, Tengfei Pang, Leilei Yan, Xuehong Wei, Jianbin Chao, Chanjuan Xi
Summary: An efficient and highly selective C-O bond cleavage of N-methylated formanilides is achieved by using NaBH4 as the reductant under CO2 tuning. The mechanism is proposed based on detailed investigations of the role of CO2 in the reaction.
Article
Chemistry, Physical
Ying Wang, Wei Zeng, Yanfei Zhao, Minhao Tang, Xiaoqian Chang, Yueting Xu, Rongxiang Li, Zhimin Liu
Summary: This study presents a simple and green strategy to prepare high-performance Ru catalysts for CO2 hydrogenation using cellulose and phytic acid composite (CPC) as support. The CPC support exhibits a porous structure with abundant functional groups that can complex with Ru(III). The resulting CPC-Ru catalyst showed much higher activity and selectivity compared to reported heterogeneous Ru catalysts. Furthermore, the catalyst demonstrated good recyclability and stability after multiple runs.
Article
Chemistry, Multidisciplinary
Fengtian Wu, Yuepeng Wang, Yong Qian, Zong-Bo Xie, Zhengang Ke, Yanfei Zhao, Zhimin Liu
Summary: In this study, a green approach to produce benzyl phenyl sulfide derivatives using thioanisoles and benzyl alcohols as starting materials and the ionic liquid 1-propylsulfonate-3-methylimidazolium trifluoromethanesulfonate as the catalyst was reported. The mechanism was found to involve the activation of the starting materials by the synergistic effect of the cation and anion of the ionic liquid, leading to the formation of benzyl phenyl sulfide derivatives. This method offers a simple, efficient, and environmentally friendly way to synthesize benzyl phenyl sulfide derivatives with promising application potentials.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Pengsong Li, Jiahui Bi, Jiyuan Liu, Qinggong Zhu, Chunjun Chen, Xiaofu Sun, Jianling Zhang, Zhimin Liu, Buxing Han
Summary: In order to achieve commercial CO2 electrochemical reduction to C2+ alcohols, the selectivity and production rate need to be further improved. This study presents a room-temperature one-step synthetic strategy to fabricate a highly stable Cu aerogel as an efficient CO2 reduction electrocatalyst. The Cu aerogel obtained by reducing Cu2+ using a weak reductant showed a high selectivity for C2+ products, while the Cu aerogel prepared using a strong reductant was favorable to generating CO.
Article
Multidisciplinary Sciences
Fengtian Wu, Yuepeng Wang, Yanfei Zhao, Minhao Tang, Wei Zeng, Ying Wang, Xiaoqian Chang, Junfeng Xiang, Buxing Han, Zhimin Liu
Summary: In this study, a simple, metal-free, and efficient aminolysis strategy was developed to upcycle polylactic acid and poly(bisphenol A carbonate) into value-added chemicals. The strategy involves the use of anilines over lactate-based ionic liquids, resulting in the formation of N-aryl lactamides and bisphenol A derivatives. The activation of polyester carbonyl atoms and enhancement of aniline nucleophilicity were achieved through hydrogen bonding interactions with lactate anions. The nucleophilic attack of aniline nitrogen atoms on polyester carbonyl carbon atoms led to cleavage of the CO bond and the desired product formation.
Article
Nanoscience & Nanotechnology
Yubo Liang, Cailing Wu, Songjie Meng, Zhansheng Lu, Runyao Zhao, Huiyong Wang, Zhimin Liu, Jianji Wang
Summary: In this study, Ag single-atom catalysts (SACs) supported on CeO2 (Ag-1/CeO2) were prepared using a new in situ adsorption-reduction method. The Ag single atoms were anchored on CeO2 through strong metal-support interaction (SMSI) and were accompanied by three interfacial oxygen vacancies. Ag-1/CeO2 exhibited high performance in the electrocatalytic CO2 reduction reaction (CO2RR), with a high CO faradaic efficiency (FE) of >95% and a turnover frequency (TOF) value of 50,310 h(-1) at FECO = 99.5% in H-cells. Notably, Ag-1/CeO2 achieved an industrial-grade current density of 403 mA cm(-2) with a high FECO of 97.2% in flow cells. Experimental results and density functional theory calculations revealed that the superior performance was mainly attributed to the existence of interfacial oxygen vacancies, which formed Ag-O-Ce3+ atomic interfaces and activated the Ce3+-O structures as the synergistic active center of Ag, thereby promoting CO2 adsorption and activation and reducing the reaction potential barrier of *COOH-to-*CO.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Zhengang Ke, Yuepeng Wang, Yanfei Zhao, Minhao Tang, Wei Zeng, Ying Wang, Xiaoqian Chang, Buxing Han, Zhimin Liu
Summary: In this study, an ionic-liquid (IL) hydrogen-bonding promoted dihydrogen auto-transfer strategy was used for the amination of alcohols to higher amines over a cobalt catalyst under base-free conditions. The strategy demonstrated high performance and tolerance to a wide range of amines and alcohols, resulting in good to excellent yields of higher amines. The mechanism investigation suggested that the [BF4] anion played a key role in activating the alcohol and facilitating the transfer of hydrogen atoms to the cobalt catalyst, leading to the formation of aldehyde intermediates and cobalt dihydride complexes, which were involved in the subsequent reductive amination. This green and effective route for alcohol amination has potential applications in alcohol-involved alkylation reactions.
Article
Chemistry, Multidisciplinary
Pengsong Li, Jiahui Bi, Jiyuan Liu, Yong Wang, Xinchen Kang, Xiaofu Sun, Jianling Zhang, Zhimin Liu, Qinggong Zhu, Buxing Han
Summary: CuGa catalyst promotes efficient electrocatalysis of CO2 to C2+ products at high current density through p-d orbital hybridization. The p-d hybridization of Cu and Ga enriches reactive sites, enhances the binding strength of the *CO intermediate, and facilitates C-C coupling. This strategy can be extended to other p-block metal-doped Cu catalysts to further enhance CO2 electroreduction for C2+ production. This is the first study to utilize p-d orbital hybridization interaction in a p block metal-doped Cu catalyst to promote electrochemical CO2 reduction to generate C2+ products.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Qian Zhang, Shuaiqi Gao, Yingying Guo, Huiyong Wang, Jishi Wei, Xiaofang Su, Hucheng Zhang, Zhimin Liu, Jianji Wang
Summary: Cobalt coordinated covalent organic frameworks have shown promise for CO2 photoreduction to CO, but achieving high conversion efficiency is challenging due to fast recombination of electron-hole pairs. This study designs Co-COF catalysts with oxygen coordinated Co atoms, and the reported Co-O-4 sites significantly enhance carrier migration and inhibit recombination, resulting in a high CO production rate of 18000 μmol g(-1) h(-1) and 95.7% selectivity under visible light irradiation. This work opens up new possibilities for designing high-performance catalysts for CO2 photoreduction.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Jiahui Bi, Pengsong Li, Jiyuan Liu, Shuaiqiang Jia, Yong Wang, Qinggong Zhu, Zhimin Liu, Buxing Han
Summary: By using a 3D copper-chitosan gas diffusion layer electrode, efficient conversion of carbon dioxide to C2+ alcohols at high current density can be achieved. This electrode structure facilitates rapid electron transport, mitigates mass diffusion limitations, and exhibits high selectivity and Faradaic efficiency for C2+ alcohols under optimal conditions.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ruipeng Li, Xing Zhou, Zhiyong Li, Yuepeng Wang, Yanfei Zhao, Zhimin Liu, Changling Yan, Cailing Wu, Yang Zhao, Jianji Wang
Summary: Selective intramolecular dehydration of biomass-derived cyclic alcohols to cyclic alkenes is achieved via cation- and anion-confined catalysis over Lewis acid imidazolium-Zn based ionic liquids. The [BMIm][Zn2Cl5] catalyst provides a confined microenvironment for the coordination of Zn2+ with hydroxyl O of cyclic alcohols, leading to exclusive intramolecular dehydration. The strategy offers a promising alternative for the green synthesis of cyclic alkenes from renewable biomass-derived alcohols.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Xiaoqian Chang, Yuepeng Wang, Yanfei Zhao, Ying Wang, Rongxiang Li, Zhengang Ke, Penglei Chen, Zhimin Liu
Summary: A simple and green approach for the synthesis of 1,4-dioxanes using hydrogen-bonding catalysis in ionic liquids has been developed.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Huan Wang, Zhi-Hao Zhao, Yanfei Zhao, Fengtao Zhang, Junfeng Xiang, Buxing Han, Zhimin Liu
Summary: In this study, a novel and green catalytic strategy was proposed for the ring-closing metathesis of alkoxy alcohols to form cyclic ethers under metal-free conditions. The use of a cation-anion confined hydrogen bonding catalyst showed high activity and recyclability, allowing for the synthesis of a wide range of O-heterocycles.
Article
Chemistry, Multidisciplinary
Huan Wang, Zhi-Hao Zhao, Yanfei Zhao, Fengtao Zhang, Junfeng Xiang, Buxing Han, Zhimin Liu
Summary: Researchers proposed a new catalytic strategy using cation-anion confined hydrogen bonding to catalyze the ring-closing metathesis of alkoxy alcohols, leading to the synthesis of cyclic ethers.
