Article
Chemistry, Multidisciplinary
Kyle J. Korman, Michael R. Dworzak, Glenn P. A. Yap, Eric D. Bloch
Summary: This paper describes the preparation of a new class of reactive porous solids through straightforward salt metathesis reactions. A porous solid is obtained by reacting the dimethylammonium salt of a magnesium-based porous coordination cage with the chloride salt of [(CrCl)-Cl-II(Me(4)cyclam)](+), with simultaneous removal of dimethylammonium chloride. The porous salt exhibits a Brunauer-Emmett-Teller (BET) surface area of 213 m(2) g(-1) and the chromium(II) cations in the structure are still accessible and reactive, as confirmed by UV-vis spectroscopy. The site-isolated reactive centers show enhanced stability and reactivity compared to dissolved ions.
Article
Chemistry, Multidisciplinary
Li-Li Ling, Weijie Yang, Peng Yan, Min Wang, Hai-Long Jiang
Summary: This study presents the synthesis of Pd3Cu@UiO-66 for CO2 hydrogenation to methanol. Under light irradiation, Pd3Cu@UiO-66 exhibits a higher methanol production rate, attributed to the photo-induced electron transfer and the proximity between CO2 and H2 activation sites in the Pd3Cu microenvironment.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Zhiming Cui, Ting Fan, Liyu Chen, Ruiqi Fang, Chuanmao Li, Yingwei Li
Summary: A solvent assisted ligand exchange-hydrogen reduction strategy was used to selectively encapsulate ultrafine metal nanoparticles (Pd or Pt) within the shallow layers of MOF UiO-67. By controlling the conditions, the particle sizes of the encapsulated nanoparticles and the thickness of the embedded layers can be easily adjusted. Compact encapsulation of nanoparticles within the shallow layers of MOFs can enhance catalytic efficiency and utilization.
SCIENCE CHINA-CHEMISTRY
(2021)
Article
Chemistry, Applied
Ruiqi Fang, Liyu Chen, Zirong Shen, Yingwei Li
Summary: By utilizing hierarchical porous H-UiO-66 as a support, a series of transition-metal catalysts were synthesized for efficient conversion of furfural to furfuryl alcohol. The unique nanoarchitecture of the catalyst resulted in low mass diffusion resistance, high accessibility of metal active sites, and high durability in the liquid phase reaction, achieving nearly quantitative yield of furfuryl alcohol within 3 hours.
Article
Chemistry, Multidisciplinary
Shan-Shan Fu, Qiang-Qiang Yuan, Lihua Ma, Zhi-Ming Zhang, Tong-Bu Lu, Song Guo
Summary: A series of TEMPO@PCN-222 composite photocatalysts were developed by coordinating different amount of 4-carboxy-TEMPO with the secondary building units of PCN-222. Visible-light irradiation enables the transfer of photogenerated holes in the highest occupied molecular orbital of PCN-222 to TEMPO, significantly increasing the photosynthesis of bioactive (iso)quinolones. With an outstanding catalytic stability and substrate tolerance, TEMPO@PCN-222 exhibits a yield of 86.7% for 1-methyl-2-quinolinone, over four times higher than PCN-222 (21.4%). This study provides a new route for constructing composite photocatalysts from abundant starting materials for efficient photosynthesis of high value-added chemicals.
Article
Chemistry, Physical
Neha Antil, Ajay Kumar, Naved Akhtar, Rajashree Newar, Wahida Begum, Ashutosh Dwivedi, Kuntal Manna
Summary: The study introduces a highly efficient, chemoselective, and reusable nickel hydride catalyst for hydrogenation of nitro and nitrile compounds under mild conditions. The catalyst, based on aluminum metal-organic frameworks, has broad substrate scope and excellent functional group tolerance, and can be recycled at least 10 times. This work highlights the potential of MOF-based single-site earth-abundant metal catalysts for practical and eco-friendly production of chemical feedstocks and biofuels.
Article
Chemistry, Multidisciplinary
Timon Schoenauer, Sabrina L. J. Thomae, Leah Kaiser, Mirijam Zobel, Rhett Kempe
Summary: The development of C-N bond formation reactions is crucial in biology and chemistry, with recent progress in 3d metal catalysis showing unique selectivity patterns. By using a novel cobalt catalyst, a catalytic C-N bond formation reaction was successfully reported, utilizing abundant and low-cost starting materials for reductive alkylation.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Longlong Geng, Wenfeng Zhou, Xiaoli Wang, Tingting Li, Andrzej P. Nowak, Zhongmin Liu, Yong-Zheng Zhang, Da-Shuai Zhang, Xiuling Zhang, Haixiang Han
Summary: In this study, a decompression-thermalization strategy was used to tune the redox and catalytic hydrogenation properties of a Cu-containing metal-organic framework (MOF). The generation of open metal sites (OMSs) significantly improved the catalytic performance in hydrogenation reactions, with experimental and theoretical results showing that OMSs endow Cu species with unique electronic properties.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
Neha Antil, Manav Chauhan, Naved Akhtar, Rajashree Newar, Wahida Begum, Jaideep Malik, Kuntal Manna
Summary: In this study, a novel Ce-UiO-Co heterogeneous catalyst is reported, which can efficiently convert methane to methanol under mild conditions with high selectivity and yield. The catalyst design is based on a metal-organic framework and involves the formation of an intermediate species in the pores of Ce-UiO-66, enabling the activation and functionalization of methane.
Article
Chemistry, Physical
Neha Antil, Manav Chauhan, Naved Akhtar, Rajashree Newar, Wahida Begum, Jaideep Malik, Kuntal Manna
Summary: This article reports the development of a highly efficient catalyst for the selective oxidation of methane to methanol under mild conditions. The catalyst, a cobalt hydroxide supported by a cerium metal-organic framework, achieves a high methanol yield and selectivity using hydrogen peroxide as the oxidant. Experimental and computational studies provide insights into the active sites and catalytic mechanism of the catalyst.
Review
Biochemistry & Molecular Biology
Francisco G. Cirujano, Rafael Luque, Amarajothi Dhakshinamoorthy
Summary: Metal-organic frameworks (MOFs) have become versatile solid materials used in various applications like gas storage, separation, sensors, and catalysis. This review focuses on the use of MOFs as solid catalysts for the Henry reaction, discussing their structural properties and active sites. Comparisons with other solid catalysts in terms of activity and structural stability are made, along with suggestions for future directions in this field.
Article
Chemistry, Physical
Xu Chen, Zhiwei Qiao, Bang Hou, Hong Jiang, Wei Gong, Jinqiao Dong, Hai-Yang Li, Yong Cui, Yan Liu
Summary: Metal-organic frameworks (MOFs) have shown great potential in heterogeneous catalysis, and the enantioselectivities of chiral MOF (CMOF) catalysts can be significantly enhanced by designing metals and ligands, resulting in improved chiral catalytic reactions.
Review
Chemistry, Multidisciplinary
Amarajothi Dhakshinamoorthy, Sergio Navalon, Ana Primo, Hermenegildo Garcia
Summary: This article provides a brief summary of the advantages of metal-organic frameworks (MOFs) as catalysts in liquid-phase and gas-phase reactions, particularly in the selective CO2 hydrogenation to CH3OH. It highlights the temperature compatibility window for MOFs in the CO2 hydrogenation process and organizes the existing literature based on the role of MOFs as active sites or support for metal nanoparticles. The flexibility in design and synthesis of MOFs to enhance catalytic activity, as well as the influence of structural defects and material crystallinity, are emphasized.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Mingchun Guo, Qiangqiang Meng, Wenyao Chen, Zheng Meng, Ming-Liang Gao, Qunxiang Li, Xuezhi Duan, Hai-Long Jiang
Summary: The chemical microenvironment modulation of metal nanoparticles can effectively address the trade-off effect between activity and selectivity in catalysis. In this study, ultrafine PdCu2 nanoparticles incorporated into covalent organic frameworks (COFs) with diverse groups were fabricated for the semi-hydrogenation of alkynes. The Cu species as the primary microenvironment greatly improved selectivity, while the functional groups as the secondary microenvironment effectively regulated activity, resulting in exceptional catalytic performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Materials Science, Multidisciplinary
Chongxiong Duan, Kuan Liang, Jiahui Lin, Jingjing Li, Libo Li, Le Kang, Yi Yu, Hongxia Xi
Summary: H-MOFs, as a popular class of crystalline porous materials with hierarchical porous structures, have been widely studied in heterogeneous catalysis. They exhibit excellent catalytic activity, selectivity, stability, and recyclability, showing great potential for future research and applications.
SCIENCE CHINA-MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Zirong Shen, Zehua Luo, Junying Chen, Yingwei Li
Summary: Using few-layered nanosheet-assembled hierarchical BiOBr nanotubes with rich oxygen vacancies (OVs) as efficient photocatalysts, the simultaneous study of charge transfer and energy transfer steps in a photoexcitation process is proposed. The optimized BiOBr photocatalyst shows improved charge carrier separation and transfer, as well as enhanced exciton generation, resulting in high efficiency for photocatalytic CO2 reduction. The dominant reactive oxygen species, singlet oxygen (O-1(2)), is identified for the first time as originating from an energy transfer process, while the minor effect of superoxide anion radical (O-center dot(2)-) is observed in the photocatalytic aerobic oxidation of sulfides.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jianmin Chen, Yajing Wang, Fengliang Wang, Yingwei Li
Summary: Controllable product selectivity in CO2 hydrogenation is achieved by light-induced switching of reaction pathways over Co decorated Pt@UiO-66-NH2. With light irradiation, the main product CO is switched to CH3OH via the formate pathway, resulting in a significantly higher space-time yield of CH3OH. Mechanism investigation reveals that excited UiO-66-NH2 can transfer electrons to Pt nanoparticles and Co sites, promoting the CO2-to-*HCOO conversion and suppressing the reverse water gas shift (RWGS) pathway.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Chenghong Hu, Yue Zhang, Anqian Hu, Yajing Wang, Xiaoming Wei, Kui Shen, Liyu Chen, Yingwei Li
Summary: A strategy of synergistically near- and long-range regulation is reported to effectively modulate the electronic structure of single-atom sites. ZnN4S1/P-HC exhibits excellent performance for CO2 reduction reaction (CO2RR) with a Faraday efficiency of CO close to 100%. The coupling of CO2RR with hydrazine oxidation reaction in a two-electrode electrolyzer can greatly lower the cell voltage, theoretically saving 46% of energy consumption.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wen Yao, Anqian Hu, Jieting Ding, Nanshu Wang, Ze Qin, Xianfeng Yang, Kui Shen, Liyu Chen, Yingwei Li
Summary: An etching-functionalization strategy was developed to construct a tannic-acid-functionalized MOF with a unique hollow-wall and 3D-ordered macroporous structure. This MOF can be further used as a precursor for the synthesis of cobalt supported on oxygen/nitrogen co-doped carbon composites with H-3DOM structures and hydrophilic surface. The resulting catalyst exhibits high electrocatalytic activity in the oxygen reduction reaction.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yu Xin, Kui Shen, Tongtian Guo, Liyu Chen, Yingwei Li
Summary: This study explores the use of a metal-organic framework templated pyrolysis strategy to prepare cobalt/nitrogen-codoped carbon nanosheet arrays on carbon cloth as efficient and low-cost bifunctional electrocatalysts for seawater electrolysis. The optimized electrocatalyst shows remarkable reduction in energy consumption and prevents undesired anodic corrosion caused by chlorine oxidation reaction. It achieves high efficiency in hydrazine-assisted water electrolysis system for hydrogen production.
Article
Chemistry, Physical
Yajing Wang, Jianmin Chen, Liyu Chen, Yingwei Li
Summary: This study reports the design of ZrO2-anchored dual-atom Pt-Ni pairs for the reverse water-gas-shift (RWGS) reaction. The dual-atom material achieves a CO selectivity of 99.8% and a space-time yield of 157.2 mu molCO g(cat)(-1) s(-1) at atmospheric pressure. Theoretical calculations show that the dual-atom Pt-Ni pairs can direct the dual electronic transfer paths to efficiently activate CO2 in the RWGS reaction and enable facile desorption of the CO product.
Article
Chemistry, Physical
Ze Qin, Liyu Chen, Yingwei Li, Kui Shen
Summary: Researchers have synthesized a bifunctional catalyst with core-shell distributed ZrO2 and Co nanoparticles, which can catalyze the one-pot tandem reaction of nitroarenes with CO2 to form formamides. The catalyst exhibits high yield and good recyclability, providing valuable insights for the design of efficient catalysts for tandem CO2 fixation reactions.
Article
Chemistry, Physical
Yang Chen, Jiafeng Wu, Yingwei Li
Summary: Stepwise electrocatalytic strategy of catalysis-immobilization-deposition is proposed to achieve the consistency of diffusion and catalysis of polysulfides. A sandwich-like stepwise electrocatalyst composed of Co nanoparticles, mesoporous SiO2, and iron single atom is designed as the catalysis core, immobilization interlayer, and deposition shell, respectively. The S/Co-NP@SiO2@Fe-SA cathode delivers high reversible capacity and areal capacity, shedding light on a new host design concept for high-performance lithium-sulfur batteries.
Article
Chemistry, Multidisciplinary
Jieting Ding, Danyu Guo, Nanshu Wang, Hao-Fan Wang, Xianfeng Yang, Kui Shen, Liyu Chen, Yingwei Li
Summary: This study reports a defect engineering strategy to facilitate the structural transformation of MOFs to metal oxyhydroxides during OER, resulting in enhanced activity. Defective MOFs with abundant unsaturated metal sites are constructed, which can be more easily transformed to metal oxyhydroxides compared to non-defective MOFs. Furthermore, the metal oxyhydroxides derived from defective MOFs exhibit more oxygen vacancies, which greatly improve the OER activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Dongwen Guo, Kai Jiang, Hui Gan, Yanwei Ren, Jinxing Long, Yingwei Li, Biaolin Yin
Summary: Developing well-defined structures and desired properties for porous organic polymer (POP) supported catalysts by controlling their composition, size, and morphology is of great significance. Herein, we report a preparation of polyaniline (PANI) supported Pd nanoparticles (NPs) with controllable structure and morphology. The Pd/PANI catalysts with different charge transfer properties between Pd and PANI, as well as different dispersions of the metal NPs, greatly improve the turnover frequency (TOF) in the reductive coupling of furfural derivatives to potential bio-based plasticizers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Wenyuan Lyu, Yang Liu, Jingyi Zhou, Datong Chen, Xin Zhao, Ruiqi Fang, Fengliang Wang, Yingwei Li
Summary: Photocatalytic conversion of low-concentration CO2 is a promising way to address environmental and energy issues. In this study, oxygen vacancy contained Co3O4 hollow nanoparticles were designed and fabricated to enhance the conversion of low-concentration CO2. By breaking the local structural symmetry and creating asymmetric active sites, the binding and structural polarization of CO2 molecules were improved, leading to unprecedented activity under laboratory light source or natural sunlight.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Chemical
Xin Zhao, Ruiqi Fang, Fengliang Wang, Zirong Shen, Xianfeng Yang, Xiang-Peng Kong, Yingwei Li
Summary: A novel defect-induced strategy is used to fabricate Cu single-atom sites with unsaturated coordination configurations. Cu is stabilized using polyvinyl pyrrolidone and pores are generated in adjacent areas. The Cu atoms are distributed on C2 sites at the edge of pores in carbon support. The Cu1C2 moiety with unsaturated coordination configurations exhibits superior catalytic performance in the oxidative coupling reaction.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Xin Zhao, Ruiqi Fang, Fengliang Wang, Yingwei Li
Summary: A newly developed precise locating carbonization strategy is reported for the fabrication of 21 kinds of dual-metal single-atom catalysts with N, S co-coordinated configurations. The CoN3S1/CuN4@NC catalyst shows remarkable performance in O-2 activation and enables a spontaneous process through its dynamic configuration, significantly outperforming the CoN4/CuN4@NC and CoN3S1@NC counterparts. Hence, CoN3S1/CuN4@NC exhibits attractive performance in the domino synthesis of natural flavone and 19 kinds of derivatives.
Article
Chemistry, Physical
Jiafeng Wu, Yuanyi Feng, Yang Chen, Ting Fan, Yingwei Li
Summary: In this study, a dual-metal Zn-Co single-atom catalyst loaded on a double-shelled nitrogen-doped carbon material is designed to enable efficient confinement and catalytic conversion of lithium polysulfides. The catalyst exhibits a synergistic effect of dual-redox sites and an ingenious double-shelled structure, effectively reducing the energy barrier and diffusion of polysulfides compared to single-component counterparts. When used as a sulfur host, the catalyst shows satisfactory sulfur electrochemistry, including excellent reversible performance and superior areal capacity.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Xin Zhao, Ruiqi Fang, Fengliang Wang, Xiangpeng Kong, Yingwei Li
Summary: A versatile complexation-deposition strategy was demonstrated for the synthesis of 13 kinds of dual-metal single-atom (SA) site pairs with uniform and exclusive coordination configurations. The CuN4/CoN2P2 site pairs exhibited significantly enhanced catalytic activity and selectivity in the synthesis of natural flavonoids, attributed to the unsymmetrical electron distribution over the sites.
