Article
Chemistry, Multidisciplinary
Huoliang Gu, Guoshuai Shi, Lixiang Zhong, Lingmei Liu, Honghao Zhang, Chunlei Yang, Ke Yu, Chenyuan Zhu, Jiong Li, Shuo Zhang, Chen Chen, Yu Han, Shuzhou Li, Liming Zhang
Summary: This study demonstrates the use of an ultrathin conjugated metalloporphyrin covalent organic framework grown on graphene as a two-dimensional van der Waals heterostructure for CO2 reduction. The strong interlayer coupling enhances the catalytic efficiency by accelerating the kinetics of CO2 conversion. The results highlight the importance of strong electronic coupling between van der Waals layers in accelerating CO2 conversion dynamics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Rajesh Patra, Debajit Sarma
Summary: Thiol-containing biomolecules, such as cysteine and glutathione, have important roles in regulating polarity and reactivity. Thiol MOFs, a subclass of functional MOFs, are relatively unexplored due to synthetic challenges and stability and storage issues. However, they have advantages due to the reactivity and affinity of the thiol groups with soft metal ions. In this study, a thiol MOF was functionalized with silver ions to create a silver nanoparticle-functionalized heterogeneous catalyst (Ag@Zr-DMBD), which showed efficient CO2 fixation to cyclic carbonates under mild conditions.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Shuo Liu, Ming-Liang Gao, Chen-Ning Li, Lin Liu, Zheng-Bo Han
Summary: A general approach to prepare superhydrophobic MOFs-CF3 through a post-decorating strategy for highly efficient chemical fixation of CO2 was demonstrated. The enhanced catalytic activity of MOFs-CF3 is attributed to a synergistic effect between the Lewis acid sites of MOFs and modification of the electron-withdrawing trifluoromethyl group, resulting in a high CO2 enrichment capacity. The possible mechanism of cycloaddition catalyzed by the MOFs-CF3 catalyst was also proposed.
DALTON TRANSACTIONS
(2023)
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.
Review
Chemistry, Inorganic & Nuclear
Xuan Zhang, Megan C. Wasson, Mohsen Shayan, Ellan K. Berdichevsky, Joseph Ricardo-Noordberg, Zujhar Singh, Edgar K. Papazyan, Anthony J. Castro, Paola Marino, Zvart Ajoyan, Zhijie Chen, Timur Islamoglu, Ashlee J. Howarth, Yangyang Liu, Marek B. Majewski, Michael J. Katz, Joseph E. Mondloch, Omar K. Farha
Summary: Porphyrins are important molecules widely found in nature, and recent interest in using them as building blocks for metal-organic frameworks has increased rapidly. Porphyrin-based MOFs with atomically precise structures provide an ideal platform for studying structure-function relationships in the solid state without compromising the inherent properties of the porphyrin building blocks.
COORDINATION CHEMISTRY REVIEWS
(2021)
Review
Nanoscience & Nanotechnology
Adrien Schlachter, Paul Asselin, Pierre D. Harvey
Summary: Porphyrin-based or porphyrin-containing metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs) have shown promise as heterogeneous photosensitizers for generating singlet oxygen in a photoredox process, with potential applications in antimicrobial treatments.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Yefei Wang, Liang Zhao, Guanfeng Ji, Cheng He, Songtao Liu, Chunying Duan
Summary: In this study, the inert C(sp(3))-H bond activation was achieved by stabilizing the active tertbutyl peroxide radical with vanadium(V-IV)-porphyrin-based metal-organic frameworks (MOFs) and utilizing a synergistic bimetallic strategy via a hydrogen atom transfer process. The introduction of {Mn-3(mu(3)-O)} cluster nodes into MOFs resulted in the pre-activation of substrates, leading to enhanced conversion efficiency and product selectivity for inert C(sp(3))-H bond functionalization.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Jiangnan Li, Gemma L. Smith, Yinlin Chen, Yujie Ma, Meredydd Kippax-Jones, Mengtian Fan, Wanpeng Lu, Mark D. Frogley, Gianfelice Cinque, Sarah J. Day, Stephen P. Thompson, Yongqiang Cheng, Luke L. Daemen, Anibal J. Ramirez-Cuesta, Martin Schroder, Sihai Yang
Summary: Reversible high-capacity adsorption of SO2 has been achieved in Zr-based metal-organic framework (MOF) materials. By introducing amine, atomically-dispersed Cu-II, or heteroatomic sulphur sites into the pores, the capture of SO2 at low concentrations is enhanced, and the captured SO2 can be converted to a valuable pharmaceutical intermediate.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
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
Multidisciplinary Sciences
Shaghayegh Naghdi, Alexey Cherevan, Ariane Giesriegl, Remy Guillet-Nicolas, Santu Biswas, Tushar Gupta, Jia Wang, Thomas Haunold, Bernhard Christian Bayer, Gunther Rupprechter, Maytal Caspary Toroker, Freddy Kleitz, Dominik Eder
Summary: In this study, the authors demonstrate that selective ligand removal in metal-organic frameworks (MOFs) can introduce new active sites and mesopores, leading to enhanced photocatalytic hydrogen evolution. This strategy allows for the purposeful engineering of hierarchical MOFs, advancing their applicability in environmental and energy technologies.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Luis Leon-Alcaide, Javier Lopez-Cabrelles, Maria Esteve-Rochina, Enrique Orti, Joaquin Calbo, Bas Huisman, Michele Sessolo, Joao Waerenborgh, Bruno Vieira, Guillermo Minguez Espallargas
Summary: Bond breaking is a new tool for postsynthetically modifying the pore structure in metal-organic frameworks. In this study, the concept of clip-off chemistry is extended to ZIF-8, and the different stabilities of bonds between imidazolate and Zn and Fe metal atoms in heterometallic Fe-Zn-ZIF-8 are utilized. It is demonstrated that Fe centers can be selectively removed without affecting the backbone structure supported by Zn atoms. This strategy allows for the creation of mesopores within the highly stable ZIF-8 structure and opens up new possibilities for designing novel hierarchical porous frameworks.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Zhenzhen Zhou, Xiao Liu, Jian-Gong Ma, Peng Cheng
Summary: Environmental problem caused by carbon emission has attracted widespread attention. This study developed a new dual-active site catalyst for converting CO2 into formamides, which has the advantages of high efficiency, low cost, and reusability. It provides a reliable approach to unify the advantages of homogeneous and heterogeneous catalysts, and has significant implications for synthetic chemistry and environmental protection.
Article
Engineering, Chemical
Zhengdong Guo, Yijian Li, Peixin Zhang, Jiyu Cui, Liyuan Chen, Lifeng Yang, Jun Wang, Xili Cui, Huabin Xing
Summary: A highly-stable ultramicroporous material CPL-1-NH2 was reported for efficient separation of low concentration SO2 and CO2, with high separation selectivity. The narrow channel with lined amino groups in this material exhibits significantly higher affinity to SO2 than CO2, demonstrating good capture performance even in the presence of CO2 and trace moisture.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Multidisciplinary Sciences
Yifan Gu, Jia-Jia Zheng, Ken-ichi Otake, Shigeyoshi Sakaki, Hirotaka Ashitani, Yoshiki Kubota, Shogo Kawaguchi, Ming-Shui Yao, Ping Wang, Ying Wang, Fengting Li, Susumu Kitagawa
Summary: The authors developed a flexible porous coordination polymer (PCP) and created a corrugated channel system that selectively responds to CO2 molecules over nine other similar gas molecules. This exclusive discrimination gating (EDG) effect is achieved through framework dynamics, guest diffusion, and interaction energetics. The resulting PCP demonstrates efficient CO2 capture from various gas mixtures.
NATURE COMMUNICATIONS
(2023)
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
Nanoscience & Nanotechnology
Shao-Zhe Yi, Bao-Ning Li, Peng-Yan Fu, Mei Pan, Cheng-Yong Su
Summary: A new method for synthesizing pure organic photoluminescent molecules with dual excited-state intramolecular proton transfer (ESIPT) sites was developed. These molecules can emit full-color light from blue, green, and yellow to red, and even white light, depending on the solvents used. The study verified the dual-ESIPT mechanism through experiments on copper ions' selective photoluminescent response and solid-state photoluminescent changes upon the stimulus of organic vapor. Theoretical analysis further supported the experimental results and provided insights for the design and application of advanced dual-ESIPT optical materials.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Mei-Juan Wei, Xian-Yan Xu, Jia-Qi Song, Mei Pan, Cheng-Yong Su
Summary: A thermally stable two-dimensional cobalt-based metal-organic framework (Co-TBAPy) with superior CO2 adsorption capability and adjustable composition is synthesized for photocatalytic CO2 reduction to syngas. The proportion of CO : H-2 can be precisely regulated, enabling the synthesis of methanol and methane.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Zhifang Su, Yucheng Luo, Jianying Shi, Jianxin Feng, Xuan Li, Jinzhong Zhang, Chengyong Su
Summary: The host-guest interaction and microenvironment around the Re complex in two metal-organic frameworks, ZIF-8 and UiO-66, were investigated. It was found that ZIF-8 provided a confined space for Re through electrostatic interaction, while UiO-66 offered a relaxed space through coordination interaction. The Re@ZIF-8 exhibited a significantly higher turnover number for CO2 photoreduction compared to Re@UiO-66, which was attributed to the promotion of electron transfer in Re@ZIF-8 and hindrance in Re@UiO-66. The spatial confinement in Re@ZIF-8 stabilized charged intermediate species during CO2 activation, whereas Re-triethanolamine adducts prevailed in Re@UiO-66 due to the accessibility of the Re complex. This study demonstrates the feasibility of altering CO2 activation pathway through the microenvironment of a molecular catalyst in artificial photosynthesis.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Xiao-Hong Xiong, Zhang-Wen Wei, Wei Wang, Liu-Li Meng, Cheng-Yong Su
Summary: In this study, a viable synthetic protocol was developed to produce DUT-67 with controllable MOF structure, excellent crystallinity, adjustable shape/size, and large-scale production. Simple HCl post-treatment resulted in depurated DUT-67-HCl with ultrahigh purity, excellent chemical stability, fully reversible SO2 uptake, and high separation selectivity. This research has important implications for future SO2 capture and recovery technology.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Huanfeng Huang, Shunlian Ning, Yanyu Xie, Zhujie He, Jun Teng, Zhuodi Chen, Yanan Fan, Jian-Ying Shi, Mihail Barboiu, Dawei Wang, Cheng-Yong Su
Summary: Researchers have developed a new trimetallic Fe-Co-Ni hydroxide electrocatalyst with a nanotubular structure through an enhanced Kirkendall process under applied potential. This FeCoNiOxHy catalyst exhibits synergistic electronic interaction between Fe, Co, and Ni, leading to increased intrinsic activity and conductivity. As a result, FeCoNiOxHy shows remarkably accelerated OER kinetics and superior apparent activity. This work is of fundamental and practical significance for advanced energy conversion materials and technologies.
Article
Multidisciplinary Sciences
Huai Chen, Yangyang Xiong, Jun Li, Jehad Abed, Da Wang, Adrian Pedrazo-Tardajos, Yueping Cao, Yiting Zhang, Ying Wang, Mohsen Shakouri, Qunfeng Xiao, Yongfeng Hu, Sara Bals, Edward H. H. Sargent, Cheng-Yong Su, Zhenyu Yang
Summary: This study reports an epitaxial growth method to construct Co single atoms on Si for light-driven CO2 reduction to syngas. By improving the dispersion of active sites and the efficient harvest of photons, the cobalt-on-silicon single-atom catalysts achieved a 10% external quantum efficiency for CO2-to-syngas conversion, with tunable H2/CO ratio between 0.8 and 2. This photocatalyst also achieved a turnover number of 2 x 10(4) for visible-light-driven CO2 reduction over 6 hours, which is over ten times higher than previously reported single-atom photocatalysts.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Zheng Wang, Xiao-Yu Zhang, Jun-Ting Mo, Cheng-Yong Su, Mei Pan
Summary: A new strategy using metal-organic complex (MOC) cations as the organic components is proposed to create a novel type of organic-inorganic perovskitoid material. The synthesized lead-free MOC-inorganic perovskitoid exhibits tunable fluorescence color and achieves cold white light emission. The material also shows bright and color-tunable long persistent luminescence even after the removal of the radiation source.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Jia-Qi Song, Yu-Lin Lu, Shao-Zhe Yi, Jian-Hua Zhang, Mei Pan, Cheng-Yong Su
Summary: Photocatalytic reduction of excess CO2 in the atmosphere to value-added chemicals by visible light can be achieved using a trinuclear Re(I)-coordinated organic cage (Re-C-4(R)) as the supramolecular photocatalyst. The Re-C-4(R) exhibits higher catalytic activity and CO2 adsorption ability compared to its mononuclear analogue Re-bpy, due to its covalent linkage, cryptand structure, and multiple amine groups. The trinuclear cryptate structure of Re-C-4(R) also facilitates electron transfer efficiency during CO2 reduction, as indicated by its shorter decay lifetimes in transient absorption and photoluminescence decay spectra compared to Re-bpy.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Xin Zhao, Bing-Bing Qin, Tao He, Hai-Ping Wang, Jiewei Liu
Summary: A pyrene-based metal-organic framework, Cd-2(PTTB)(H2O)(2) (WYU-11), was synthesized and found to exhibit stability in various environments. It showed excellent catalytic performance in the cyclization reaction of propargylic amines with CO2 and demonstrated outstanding water stability and luminescence properties for detection of sulfathiazole and ornidazole.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Peng-Yan Fu, Shao-Zhe Yi, Mei Pan, Cheng-Yong Su
Summary: In recent years, metal-organic supramolecular optical materials have attracted great attention due to their adjustable frame structures, diverse emission types, and excellent optical performance. By regulating the equilibrium and transformation relationship of various photophysical processes, these materials demonstrate rich luminescence mechanisms and wide applications. However, there is still a lack of deep understanding on the properties of metal-organic supramolecular materials based on excited-state intramolecular proton transfer (ESIPT), and new strategies for regulating luminescence mechanisms need to be established.
ACCOUNTS OF MATERIALS RESEARCH
(2023)
Article
Chemistry, Applied
Wenqian Yang, Ziqian Xue, Jun Yang, Jiahui Xian, Qinglin Liu, Yanan Fan, Kai Zheng, Peiqin Liao, Hui Su, Qinghua Liu, Guangqin Li, Cheng-Yong Su
Summary: Selective electrochemical reduction of CO2 to CO remains challenging due to the competing hydrogen evolution reaction. In this study, N-doped sponge-like porous graphitic carbon structures embedded with Fe nanoparticles (Fe@NPC) were fabricated and showed a high CO Faradaic efficiency of 96.4% and good stability. This outstanding CO2 reduction performance was attributed to the unique structure of Fe@NPC, which provided abundant hierarchical pores for CO2 adsorption and mass transfer, as well as active Fe sites that accelerated CO generation kinetics. Fe@NPC also exhibited improved ability to accumulate the crucial intermediate *COOH compared to other pyrolyzed porous carbons. Fe@NPC was further utilized in a Zn-CO2 battery, demonstrating its potential for energy-converting devices.
CHINESE JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Zhujie He, Huanfeng Huang, Zhuodi Chen, Yuqian Liang, Zhixiang Huang, Shunlian Ning, Lilin Tan, Mihail Barboiu, Dawei Wang, Cheng-Yong Su
Summary: Catalytic CO2 methanation has significant applications in various industrial fields, and the development of advanced heterogeneous catalysts for this process is challenging. In this study, we developed a TiH2-supported Ru catalyst with enhanced CO intermediate activation capability. The optimized catalyst exhibited notable CH4 selectivity and production rate, surpassing pure Ru nanoparticles. This work provides valuable insights for the development of highly efficient CO2 conversion catalysts.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Liang Zhang, Xiao-Hong Xiong, Liu-Li Meng, Lu-Zhu Qin, Cheng-Xia Chen, Zhang-Wen Wei, Cheng-Yong Su
Summary: A pore-nanospace-engineering strategy was used to construct UiO-66-type zirconium MOFs with different aromatic linkers for natural gas separation and purification. The introduction of naphthalene moieties in UiO-66-Naph showed the best potential for separating C2/C3 (C2H6 and C3H8) light hydrocarbons from CH4.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Inorganic & Nuclear
Chunying Chen, Qijie Mo, Yufei Wang, Li Zhang
Summary: Vinylsilanes are important structural units in organic chemistry. This study reports a catalytic alkyne hydrosilylation method using a porphyrin metal-organic framework with incorporated Pd nanoparticles. The catalytic results show that the catalyst has high efficiency and selective production of E isomer vinylsilane. Mechanistic studies reveal that the cooperation between iridium porphyrin and Pd nanoparticles is the key to the high catalytic activity.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jieli Lin, Shihua Liu, Jie Zhang, Hansjorg Grutzmacher, Cheng-Yong Su, Zhongshu Li
Summary: In this study, N-heterocyclic vinyl (NHV) substituted diphosphenes were isolated and characterized as both E- and Z-isomers. The thermodynamically more stable E-2b undergoes reversible photo-stimulated isomerization to Z-2b, which can be thermally reverted back to E-2b. The study also reveals the coordination of both E- and Z-2b to an AuCl fragment, as well as their different cycloaddition reactions.
