Article
Chemistry, Physical
Julia S. Schulze, Raoul D. Brand, Joachim G. C. Hering, Luise M. Riegger, Peter R. Schreiner, Bernd M. Smarsly
Summary: In this study, the immobilization of 4-dimethylaminopyridine (DMAP) on mesoporous silica particles and macro-mesoporous silica monoliths for continuous flow synthesis was reported. The immobilized DMAP derivatives were characterized and their catalytic performance was studied. The results showed that both materials achieved high conversion rates in continuous flow experiments, with the macro-mesoporous silica monoliths exhibiting lower pressures and higher turnover rates compared to packed bed reactors.
Article
Chemistry, Applied
Yang Li, Jing Wang, Sisi Fan, Fanan Wang, Zheng Shen, Hongmin Duan, Jinming Xu, Yanqiang Huang
Summary: Spherical carbon beads with effective CO2 capture capability were synthesized via co-pyrolyzation of poly(vinylidene chloride) and melamine, resulting in nitrogen-doped hierarchically porous carbon spheres. These carbon spheres exhibited outstanding CO2 capture performance due to their enriched nitrogen functionalities and special hierarchical porous structure.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Physical
Cristian Rosso, Sara Cuadros, Giorgia Barison, Paolo Costa, Marina Kurbasic, Marcella Bonchio, Maurizio Prato, Luca Dell'Amico, Giacomo Filippini
Summary: We present an efficient photocatalytic method for the direct iodosulfonylation of terminal olefins using alpha-iodo phenylsulfones. The process utilizes a phenol derivative as the precatalytic system and visible-light irradiation. Mechanistic investigations demonstrate the crucial role of the in situ generated phenolate anion in the catalytic process, achieving high yields of up to 95%.
Review
Chemistry, Inorganic & Nuclear
Lin Zhang, En-Qing Gao
Summary: Carbon dioxide (CO2) is a dominant greenhouse gas and a plentiful and renewable C1 resource. This article reviews the recent research on the chemical fixation and conversion of CO2 to high-value chemicals, with a focus on the direct carboxylation of C(sp)-H bonds. The use of metal catalysts, both homogeneous and heterogeneous, as well as the emerging field of organocatalysis, is discussed in detail.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Physical
Anna Lenarda, Michele Melchionna, Santeri Aikonen, Tiziano Montini, Paolo Fornasiero, Tao Hu, Michael Hummel, Juho Helaja
Summary: Activated carbons obtained from organosolv lignin were used as catalysts for aerobic oxidative dehydrogenation (ODH) reactions. The relationship between structure and activity was investigated, and the distribution of oxygen functionality was found to play a crucial role. The catalytic activity was associated with C=O surface functionalities, which was confirmed by blocking experiments. The breadth of the catalysts' applicability was explored through selected relevant ODH reactions.
Article
Nanoscience & Nanotechnology
Miguel Sanchez-Fuente, Alberto Lopez-Magano, Alicia Moya, Ruben Mas-Balleste
Summary: Condensation of BINAPO-(PhCHO)(2) and 1,3,5-tris(4-aminophenyl)benzene(TAPB) leads to a new imine-based chiral organic material (COM) that can be post-functionalized through reductive transformation of imine linkers to amines. Although the imine-based material is not stable enough to be used as a heterogeneous catalyst, the reduced amine-linked framework can be efficiently utilized in asymmetric allylation of various aromatic aldehydes. The obtained yields and enantiomeric excesses are comparable to those observed for the molecular BINAP oxide catalyst, with the added advantage of recyclability offered by the amine-based material.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Jeffrey S. Johnson, William R. Cassels, Evan T. Crawford
Summary: A simple catalytic crystallization-driven enantio- and diastereoselective Mannich reaction was disclosed for the synthesis of stereodefined alpha-monosubstituted-keto esters, dissymmetric diesters, dissymmetric diketones, and keto amides that productively leveraged product epimerization in solution. Mechanistic studies suggested that the initial enantioselective, diastereodivergent skeletal assembly was catalyzed by a chiral tertiary amine organocatalyst, which then facilitated second stage crystallization-induced diastereoconvergence to provide the challenging alpha-stereocenter in excellent stereoselectivity.
Article
Chemistry, Multidisciplinary
Arindam Modak, Anindya Ghosh, Akshay R. Mankar, Ashish Pandey, Manickam Selvaraj, Kamal Kishore Pant, Biswajit Chowdhury, Asim Bhaumik
Summary: Metal-free catalysis is challenging in green and sustainable chemistry, but solid-supported heterogeneous organocatalysts show potential in addressing metal leaching and sustainability issues. Porous organic materials are considered promising solid organocatalysts due to their robust structure and catalytic sites characteristics.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Nanoscience & Nanotechnology
Peng-Fei Mu, Lin Zhang, Ran Bu, Li-Fei Xiong, Ya-Wei Liu, En-Qing Gao
Summary: In this article, triaminoguanidine-derived covalent organic frameworks (COFs) were used as platforms to develop heterogeneous organocatalysts for C(sp)-H carboxylation. The COFs with guanidine cores and pyrazine linkers showed high catalytic performance due to the cooperation between cores and linkers. The core, deprotonated to the guanidinato group, binds and activates CO2, while the pyrazine linker activates the C(sp)-H bond through hydrogen bonding. The COFs also exhibited acid- and base-responsive chromic behaviors, making them potential materials for sensing and switching applications.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Applied
Yi Guo, Cheng Qian, Yinglong Wu, Liu Jiawei, Xiaodong Zhang, Dongdong Wang, Yanli Zhao
Summary: This review summarizes the recent research development of porous catalytic membranes for CO2 conversion, including methods such as electrocatalysis, photocatalysis, photoelectrocatalysis, thermalcatalysis, and biocatalysis.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Organic
Taiki Mori, Ryuichi Nishiyori, Sao Sumida, Yasuaki Furuya, Seiji Shirakawa
Summary: The development of efficient CO2 utilization reactions has attracted significant attention, but the research on catalytic enantioselective CO2 utilization for fine chemicals is still limited. There have been excellent methods reported using chiral metal complex catalysts, as well as organocatalyzed approaches. This review focuses on recent advances in catalytic enantioselective CO2 utilization reactions using chiral organocatalysts and provides a forecast for future research.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Muhammad Sohail, Fujie Tanaka
Summary: The DYKAT reactions can transform dihydrobenzofuranone derivatives into spirooxindole derivatives with high enantioselectivities and yields, regardless of the stereochemistry of the starting materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Nilakshi Devi, Caroline K. Williams, Ashwin Chaturvedi, Jianbing ''Jimmy'' Jiang
Summary: The study introduces an iron porphyrin catalyst, FePEG8T, which shows excellent activity, stability, and selectivity in electrocatalytic reduction of CO2 to CO. Control experiments confirm the contribution of triazole units on high catalytic activity. Long-term electrolysis demonstrates high catalyst stability.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Yi Liu, Ying Chen, Yunli Liu, Zewen Chen, Huan Yang, Zhongxiao Yue, Qing Fang, Yunfei Zhi, Shaoyun Shan
Summary: Solar energy is considered the cleanest, cheapest, and most sustainable energy source. By using Zn and N co-doped porous carbon nanosheets as catalysts and photothermal materials, the cycloaddition of CO2 can be driven efficiently with high yields. This approach offers recycling capability and exhibits high activity towards other epoxides.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Organic
Inbal L. Zak, Santosh C. Gadekar, Anat Milo
Summary: The application of secondary-sphere interactions in catalysis, inspired by the microenvironment of metalloprotein active sites, allows for deliberate orientation of reaction components and control over reactivity and selectivity. This interaction, although less common in organocatalysis, can play a decisive role in influencing catalytic outcomes.
Review
Chemistry, Multidisciplinary
Yanpei Song, Joshua Phipps, Changjia Zhu, Shengqian Ma
Summary: Water pollution poses a growing threat to humanity due to widespread contamination. Efforts have been made to purify polluted water by removing hazardous components, but conventional methods have limitations in uptake capacity and selectivity. Advanced porous materials (APMs) show promise in improving the segregation of contaminants, with their high surface area and versatility making them ideal for designing novel adsorbents. This review summarizes the development and application of APMs in various water treatments, along with assessments of adsorption performance. Future opportunities for APMs in water purification are also discussed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Yi Xie, Zeyu Liu, Yiyun Geng, Hao Li, Ning Wang, Yanpei Song, Xiaolin Wang, Jing Chen, Jianchen Wang, Shengqian Ma, Gang Ye
Summary: This review examines the recent advancements in uranium extraction from seawater, focusing on the development of adsorbents and the challenges faced in marine environments. It highlights the use of electrochemical and photochemical strategies and summarizes the latest achievements in marine testing by different countries. The review also discusses the fundamental, technical, and engineering aspects of uranium extraction from seawater, providing insights into the challenges and future prospects.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Polymer Science
Pui Ching Lan, Yin Zhang, Weijie Zhang, Xueying Ge, Shengqian Ma
Summary: Covalent organic frameworks are used to create an ideal reaction environment for hydrolysis, improving stability and efficiency.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Weijie Zhang, Zhou Lu, Lukasz Wojtas, Yu-Sheng Chen, Alexander A. Baker, Yi-Sheng Liu, Abdullah M. Al-Enizi, Ayman Nafady, Shengqian Ma
Summary: One striking feature of enzymes is their ability to trap substrates and produce shape-selective products through synergistic or cooperative binding in their enzymatic pocket. In this study, we demonstrate a targeting strategy by anchoring substrates on the internal pore wall of metal-organic frameworks (MOFs), mimicking the enzyme's ability and achieving shape-selectivity for reactions. By investigating metal metalloporphyrin-frameworks (MMPFs) with different densities and distances of binding sites, we show that the structural specificity of MMPFs allows for a facile switch in selectivity, from thermodynamically stable product to kinetic product. Thus, this proposed targeting strategy using porous materials and binding events provides a new approach for developing highly efficient heterogeneous catalysts for shifting selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yingxiang Ye, Yi Xie, Yanshu Shi, Lingshan Gong, Joshua Phipps, Abdullah M. Al-Enizi, Ayman Nafady, Banglin Chen, Shengqian Ma
Summary: Developing adsorptive separation processes using C2H6-selective sorbents is a promising alternative for energy-intensive cryogenic distillation in C2H4 purification. Our study showed that Ni-MOF 2 exhibited significantly higher performance in C2H6/C2H4 separation compared to Ni-MOF-1. The unique aromatic pore surfaces and suitable pore spaces of Ni-MOF 2 contribute to its high C2H6 uptake capacity, making it one of the best porous materials for this gas separation. It can generate 12 L kg(-1) of polymer-grade C2H4 product from equimolar C2H6/C2H4 mixtures at ambient conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Hui Yang, Mengjie Hao, Yinghui Xie, Xiaolu Liu, Yanfang Liu, Zhongshan Chen, Xiangke Wang, Geoffrey I. N. Waterhouse, Shengqian Ma
Summary: In this study, an isoreticular family of multivariate COFs with chromenoquinoline rings and electron-donating or withdrawing groups were synthesized and used as photocatalysts. The intramolecular donor-acceptor interactions in the COFs enabled tuning of charge distribution and carrier separation, leading to improved photocatalytic performance. By optimizing the optoelectronic properties, a nitro-functionalized multicomponent COF achieved a photocatalytic uranium extraction efficiency of 8.02 mg/g/day in natural seawater, surpassing all previously reported COFs. These findings demonstrate an effective design strategy for high-activity COF photocatalysts with intramolecular D-A structures not easily accessible through traditional synthetic methods.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Mengjiao Guan, Dengfeng Yang, Qing Li, Huiting Zhang, Jianan Xu, Mengmeng Cai, Weike Lin, Shengqian Ma, Qingzhi Liu
Summary: A new separation membrane was developed by superimposing two COF-based films with different aperture sizes. The double-layer superimposition membrane exhibited high water flux and salt rejection rate, overcoming the trade-off effect. The composite membrane had combined advantages of the two COF materials, with significantly higher water permeance and 100% salt rejection rate compared to conventional reverse-osmosis membranes.
APPLIED SURFACE SCIENCE
(2023)
Article
Multidisciplinary Sciences
Qing-Wei Meng, Shaochun Wu, Mingjie Liu, Qing Guo, Weipeng Xian, Xiuhui Zuo, Sai Wang, Hong Yin, Shengqian Ma, Qi Sun
Summary: Acids play a significant role in contemporary industries, but the recovery of single acids from waste streams containing various ionic species is time-consuming and environmentally unfriendly. In this study, a membrane with uniform angstrom-sized pore channels and charge-assisted hydrogen bond donors was designed to selectively conduct HCl while having negligible conductance for other compounds. The membrane exhibited exceptional selectivity for protons over other cations and for Cl- over SO42- and HnPO4(3-n)-, demonstrating prospects for HCl extraction from waste streams. These findings have implications for the design of advanced multifunctional membranes for sophisticated separation.
Article
Engineering, Environmental
Xinyi Yang, Weijin Wu, Yinghui Xie, Mengjie Hao, Xiaolu Liu, Zhongshan Chen, Hui Yang, Geoffrey I. N. Waterhouse, Shengqian Ma, Xiangke Wang
Summary: A halogenation strategy was reported to enhance the removal performance of cationic polymers for (TcO4)-Tc-99 (-) under various pH conditions. Through the introduction of halogen groups, the adsorption capacity and selectivity of the polymers were improved. This strategy allows for the efficient removal of (TcO4)-Tc-99 (-) from different waste streams and provides guidance for the design of functional adsorbents.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Abduljelili Popoola, P. S. Ghosh, Maggie Kingsland, Ravi Kashikar, D. DeTellem, Yixuan Xu, S. Ma, S. Witanachchi, S. Lisenkov, I. Ponomareva
Summary: In this study, we used first-principles density functional theory based simulations to investigate the structural, mechanical, dielectric, piezoelectric, and ferroelectric properties of 29 formate perovskites. We found that these materials exhibit highly anisotropic properties. Furthermore, we proposed and computationally characterized several formate perovskites that have not been reported yet.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Ze-Ming Xu, Zhuoyi Hu, Yali Huang, Shu-Jin Bao, Zheng Niu, Jian-Ping Lang, Abdullah M. Al-Enizi, Ayman Nafady, Shengqian Ma
Summary: Hydrogenated nitrogen heterocyclic compounds are critical in various industries. Previous studies on the partial hydrogenation of these compounds have focused on costly and toxic precious metal catalysts. This research introduces a novel P/B type MOF-FLP catalyst achieved through a solvent-assisted linker incorporation approach, which significantly enhances catalytic hydrogenation reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xiaolu Liu, Yinghui Xie, Yang Li, Mengjie Hao, Zhongshan Chen, Hui Yang, Geoffrey I. N. Waterhouse, Shengqian Ma, Xiangke Wang
Summary: This study proposes a practical approach for the selective removal of radioactive pertechnetate ions under extreme conditions. By modifying carbon capsules and utilizing an electrochemical redox process, the researchers achieved high removal capacities and excellent durability. This method offers new possibilities for nuclear waste management and environmental remediation.
Article
Chemistry, Multidisciplinary
Yin Zhang, Yao Jiang, Ayman Nafady, Zhiyong Tang, Abdullah M. Al-Enizi, Kui Tan, Shengqian Ma
Summary: The incorporation of a chiral frustrated Lewis pair into a metal-organic framework creates enzyme-mimic regions that exhibit enantio- and chemoselective hydrogenation, providing a new approach for achieving multiselectivity in heterogeneous catalysis. The enzyme-mimic region in the metal-organic framework, which features the active site of the chiral frustrated Lewis pair and auxiliary sites within its vicinity, shows excellent catalysis performance with high yields and selectivity in the hydrogenation of & alpha;,& beta;-unsaturated imines. This work not only contributes a new platform for multiselective catalysis but also opens up possibilities for developing heterogeneous catalysts with multiselectivity for challenging transformations.
ACS CENTRAL SCIENCE
(2023)
Article
Chemistry, Inorganic & Nuclear
Ling Zhang, Xi Chen, Wei-Na Wu, Xiao-Lei Zhao, Yun-Chang Fan, Yuan Wang, Zhi-Hong Xu, Ayman Nafady, Abdullah M. Al-Enizi, Shengqian Ma
Summary: An inorganic-organic hybrid probe MP-ZIF-90 was synthesized by condensation reaction between zeolitic imidazolate framework-90 (ZIF-90) and 4-methyl-1-(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl)pyridinium bromide (MP). The probe showed intense green emission and was selectively quenched by ClO- anions. It exhibited rapid (within 20 s) and sensitive response to ClO-, with a limit of detection (LOD) of 0.612 μM. Importantly, the probe was successfully applied for fluorescence imaging of ClO- anions in mitochondria of living cells and zebrafish.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Mengjie Hao, Yinghui Xie, Xiaolu Liu, Zhongshan Chen, Geoffrey I. N. Waterhouse, Hui Yang, Shengqian Ma, Xiangke Wang
Summary: Covalent organic frameworks (COFs) with photocatalytic linkers were designed for uranium extraction from seawater. A COF-based adsorption-photocatalysis strategy was developed for selective removal of uranyl from seawater without sacrificial reagents. The quaternary COF showed high uranium uptake capacity and good anti-biofouling abilities, opening the pathway for economic and efficient extraction of uranium from the oceans.