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, 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
Nanoscience & Nanotechnology
Jianwei Zheng, Liying Zhang, Yang Li, Hongbin Sun, Gang Zhang, Qi Sun
Summary: Core-shell nanocomposites with a catalytic metal-organic framework (MOF) shell are more effective and stable than bare MOF. The Fe3O4@SiO2@UiO-66 core-shell structure shows high catalytic ability and magnetic recyclability, maintaining high catalytic activity and stability over six cycles.
Review
Chemistry, Multidisciplinary
Yu Shen, Ting Pan, Liu Wang, Zhen Ren, Weina Zhang, Fengwei Huo
Summary: Metal-organic frameworks (MOFs) are widely studied in catalysis due to their flexible components, high surface area, and uniform active sites. However, the complex structures of MOFs pose challenges for researchers in selecting suitable catalysts. A programmable design strategy based on metal ions, organic ligands, modifiers, and post-treatment modules is proposed to design MOF catalysts for various reactions, enabling precise construction and regulation of their microenvironments for heterogeneous catalysis, electrocatalysis, and photocatalysis. This modular design concept offers a potent tool for exploring structure-activity relationships and accelerating the tailored design of multicomponent catalysts.
ADVANCED MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Zihao Wang, Arvin Bilegsaikhan, Ronald T. Jerozal, Tristan A. Pitt, Phillip J. Milner
Summary: Metal-organic frameworks (MOFs) are being increasingly used in synthetic chemistry as sustainable reagents and catalysts. This study systematically characterized the robustness of different MOFs towards various conditions representing synthetic organic chemistry. It found that azolate MOFs generally possess excellent chemical stabilities, while carboxylate and salicylate frameworks have complementary stabilities toward different reagents. These findings can guide the rational design of robust frameworks for synthetic chemistry applications and the development of new strategies for MOF modification.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Weijie Zhang, Ayman Nafady, Chuan Shan, Lukasz Wojtas, Yu-Sheng Chen, Qigan Cheng, X. Peter Zhang, Shengqian Ma
Summary: This study reported a novel metal-metalloporphyrin framework catalyst utilizing halogen bonding as a donor for catalyzing Diels-Alder reactions, showing high efficiency and uniqueness in facilitating organic transformations. Through experimental and computational studies, the substrate molecules were demonstrated to diffuse through the pores of the framework, establishing a host-guest system via the C-Br...pi interaction, which plays a key role in boosting catalytic efficiency. Furthermore, the unique capability of the metal-metalloporphyrin framework highlights new opportunities in using artificial non-covalent binding pockets as highly tunable and selective catalytic materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Yating Huang, Yansong Jiang, Haoqing Jin, Shujin Wang, Jianing Xu, Yong Fan, Li Wang
Summary: A new porous Co-MOF material was synthesized and showed good catalytic activity for cyanosilylation and Strecker reactions. Composite nanofiber membranes and mixed matrix membranes prepared using this material exhibited excellent reusability and catalytic activity. This provides a new strategy for developing MOF-based heterogeneous catalysts.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2023)
Review
Materials Science, Multidisciplinary
Jose-Luis Ortiz-Quinonez, Sachindranath Das, Umapada Pal
Summary: Metal ferrite nanostructures have promising prospects in catalysis and energy storage technologies, but a balanced assessment of their design, synthesis, and performance in these applications is necessary.
PROGRESS IN MATERIALS SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Wei Zhang, Michael. J. J. Bojdys, Nicola Pinna
Summary: We demonstrate a versatile synthesis strategy to combine metal-organic frameworks with nanoparticles, allowing for the formation of mono-, bi-, tri-, and quaternary composites. This method does not require specific surface structures or functionalities on the pre-formed cores. The controlled diffusion rate of alkaline vapors regulates the growth of MOFs and encapsulation of NPs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Nanoscience & Nanotechnology
Nianqiao Qin, An Pan, Jun Yuan, Fei Ke, Xiaoyan Wu, Jing Zhu, Jianqiang Liu, Junfa Zhu
Summary: Hollow core-shell catalytic nanoreactors featuring bimetallic porous Zn/Ni-MOF-2 shell and tiny Au nanoparticle core were successfully constructed through a rare crystal-structure transformation strategy. These nanoreactors exhibit outstanding multifunctional catalysis for a broad range of alcohol oxidation under the green oxidant environment, showing excellent recyclability in selective alcohol oxidation. These findings may provide a promising platform for the general construction of various metal-organic framework-based hollow core-shell nanostructures and further highly augmented catalytic applications.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Eloy P. Gomez-Oliveira, Daniel Reinares-Fisac, Lina M. Aguirre-Diaz, Fatima Esteban-Betegon, Mercedes Pintado-Sierra, Enrique Gutierrez-Puebla, Marta Iglesias, M. Angeles Monge, Felipe Gandara
Summary: This study synthesized and characterized three new bismuth metal-organic frameworks (MOFs), and demonstrated their catalytic activity in the one-pot multicomponent Strecker reaction. Among the MOFs, BiPF-7 exhibited high stability and catalytic activity, and the interaction between catalytic substrates and metal centers was analyzed through crystallography.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Organic
Giuseppe Gentile, Miriam Marchi, Michele Melchionna, Paolo Fornasiero, Maurizio Prato, Giacomo Filippini
Summary: Dual photocatalysis has become popular for functionalizing organic substrates under mild conditions. Single-atom heterogeneous catalysts (SACs) with carbon nitride-based supports have emerged as a frontier in this research field. This Concept highlights recent advances and applications of carbon nitride-based SACs in light-driven dual-catalytic processes, as well as future opportunities.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Review
Chemistry, Physical
Shuyue Jia, Dongxiao Ji, Liming Wang, Xiaohong Qin, Seeram Ramakrishna
Summary: This review introduces the research progress in the fabrication of metal-organic framework (MOF) membranes, including the preparation of pure MOF membranes and the incorporation of MOFs into polymer matrix. Through the analysis of classic cases, the advantages and disadvantages of different preparation strategies and products are compared, providing general knowledge for the needs of different application scenarios. The important role that MOF membranes play in the applications of separation, adsorption, and catalysis is highlighted, along with the opportunities and challenges in this new era.
Article
Chemistry, Multidisciplinary
Wenlei Zhang, Jichuang Wu, Wenxiong Shi, Peishan Qin, Wenfeng Lang, Xinglong Zhang, Zhida Gu, Hongfeng Li, Yun Fan, Yu Shen, Suoying Zhang, Zhongyi Liu, Yu Fu, Weina Zhang, Fengwei Huo
Summary: The article introduces a new function of metal-organic frameworks (MOFs) as an ideal model to construct structurally ordered metal promoters. The strategy of using MOFs as a model not only helps to reveal the action mechanism behind metal promoters, but also allows the anchoring of one or multiple kinds of metal promoters, especially noble metal promoters. It is demonstrated that the prepared Pd/bpy-UiO-Cu catalysts show high selectivity (>99%) in a hydrogenation reaction, thanks to the enhanced interaction between Pd nanoparticles and MOF carriers induced by Cu promoters.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Shun-Shun Qin, Ze-Kun Wang, Lei Hu, Xing-Hao Du, Zheng Wu, Maria Stromme, Qian-Feng Zhang, Chao Xu
Summary: Porous organic frameworks (POFs) with tunable structures have been widely studied in adsorption and catalysis. Introducing ionic structures into POFs enhances their functionalities for applications in metal scavenging and catalysis. This study reports a guanidinium-based ionic POF with excellent performance in palladium scavenging and heterogeneous catalysis.
Article
Nanoscience & Nanotechnology
Alvin M. H. Lim, Hua Chun Zeng
Summary: This work focuses on exploring the production of ultrathin hollow ceria or other rare-earth metal oxides, presenting a novel synthetic protocol for making ultrathin mesoporous hollow spheres with a tunable shell thickness. The approach shows promise for better utilization of rare-earth metal elements in various technological applications, including the fabrication of singular or multicomponent rare-earth metal oxides with ultrathin hollow morphology and structural uniformity.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Bowen Li, Kelvin Mingyao Kwok, Hua Chun Zeng
Summary: Zeolites, commonly used in the chemical industry, are now being synthesized and functionalized into complex hollow ZSM-5 catalysts with catalytic nanoparticles. This innovative approach enhances the stability, selectivity, and activity of the catalysts, demonstrating improved catalytic performance in hydrogenation reactions.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Polymer Science
Pei Lin Chee, Sigit Sugiarto, Yong Yu, Ying Chuan Tan, Enyi Ye, Dan Kai, Xian Jun Loh
Summary: A sustainable antioxidant carrier based on lignin is developed to deliver palmitoyl tripeptide-38, effectively addressing the issue of skin aging.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2022)
Article
Chemistry, Physical
Yu Shao, Mohammadreza Kosari, Shibo Xi, Hua Chun Zeng
Summary: Hydrogenation of CO2 to produce methanol is an important technology for reducing CO2 emissions and addressing the challenge of climate change. In this study, a Cu-ZnO/Si catalyst with superior structural and compositional properties was synthesized through carefully engineered procedures. The catalyst exhibited high selectivity in producing methanol under moderate conditions, showcasing its potential in CO2 hydrogenation.
Article
Chemistry, Physical
Ying Chuan Tan, Wei Kang Quek, Beomil Kim, Sigit Sugiarto, Jihun Oh, Dan Kai
Summary: This paper discusses the evaluation of catalysts on gas diffusion electrodes, highlighting the potential experimental factors that can influence the evaluation results and emphasizing the importance of establishing appropriate protocols.
ACS ENERGY LETTERS
(2022)
Article
Engineering, Multidisciplinary
Yihao Leow, Veronica Sequerah, Ying Chuan Tan, Yong Yu, Eric Charles Peterson, Changyun Jiang, Zheng Zhang, Le Yang, Xian Jun Loh, Dan Kai
Summary: This study develops a high-performance bioplastic from coconut husk, addressing the issues of poor mechanical performance and water stability in lignocellulosic bioplastics. By optimizing the processing conditions, the generated bioplastics exhibit strong mechanical properties and excellent water stability, making them a potential solution to replace petroleum-based plastics.
COMPOSITES PART B-ENGINEERING
(2022)
Article
Chemistry, Physical
Shenghui Zhou, Hua Chun Zeng
Summary: This study develops a new catalyst of box-like assemblies of quasi-single-layer MoS2 nanosheets, which effectively improves the selectivity for methanol synthesis and prevents excessive hydrogenation of CO2 to methane. The catalyst exhibits excellent catalytic activity and stability.
Article
Chemistry, Multidisciplinary
Chao Wang, Mohammadreza Kosari, Shibo Xi, Hua Chun Zeng
Summary: A post-synthetic strategy of inserting siliceous linkers inside metal-organic frameworks (MOFs) has been proposed to reinforce the structure and fabricate a Si-infused UiO-66 (s-UiO-66) with well-developed porosity and thermal/structural stability. This Si-infused matrix is then utilized as a catalyst host for confining ultrafine CuO nanoparticles, leading to a remarkable methanol production rate in CO2 hydrogenation reaction. This Si infusion strategy can be applied to construct stable host materials with boundary-defined structures for broadened applications under extreme circumstances.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Chemical
Alvin M. H. Lim, Hua Chun Zeng
Summary: Three different morphological variations of Zn-Al-containing layered double hydroxide (ZnAl-LDH) microspheres were synthesized and evaluated for their catalytic performance in CO2 hydrogenation to methanol. Two different Cu loading methods were employed, and it was found that the ion-exchanged catalyst exhibited better stability and performance compared to the wet impregnation catalyst. By using computational fluid dynamics simulation, it was determined that larger nanosheet spacing improved the convection-driven vortices within the LDH structure, leading to higher catalytic activities.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Review
Chemistry, Physical
Mohammadreza Kosari, Alvin M. H. Lim, Yu Shao, Bowen Li, Kelvin M. M. Kwok, Abdul Majeed Seayad, Armando Borgna, Hua Chun Zeng
Summary: Solid siliceous materials play an important role in carbon capture and utilization (CCU) by converting CO2 into valuable chemical commodities. Siliceous catalysts are widely used for CO2 thermal conversion due to their tunable porosity, high thermal resistivity, and ease of preparation. In terms of catalytic performance, siliceous-based catalysts are comparable to non-precious and precious metal catalysts. This review focuses on recent advances in CO2 conversion using silica/silicate-based catalysts, including gas-phase reduction pathways, design and synthesis techniques, and different types of catalysts. The potential for CO2 conversion to hydrocarbons, alcohols, and specialty organic substances using siliceous-based catalysts is emphasized.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Alvin Ming Hao Lim, Jun Wen Yeo, Hua Chun Zeng
Summary: A synthesis method was developed to introduce transition metal ions into MgAl-LDH using the memory effect property of calcined LDH. The resulting CuZn-doped MgAl-LDH catalyst showed high specific activity and methanol selectivity in CO2 hydrogenation. The excellent performance was attributed to the easily accessible active sites on the surface of nanostructured petals.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Bo Sun, Alvin M. H. Lim, Hua Chun Zeng
Summary: Sto''ber silica nanospheres were transformed into zinc silicate nanoflowers and used as an active catalyst for the CO2-to-MeOH reaction. The zinc silicate nanoflowers loaded with copper-(II) oxide showed excellent methanol selectivity in the reaction. This study demonstrates the potential of using these functionalized nanoflowers for efficient CO2 conversion into methanol.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Engineering, Environmental
Changwei Chen, Mohammadreza Kosari, Shibo Xi, Alvin M. H. Lim, Chi He, Hua Chun Zeng
Summary: Achieving high catalytic activity and selectivity in CO2 hydrogenation to methanol using nonprecious metals remains a challenge. Here, we spatially sequestered the ternary Cu-ZnO-ZrO2 on an engineered mesoporous silica sphere, resulting in an enhanced methanol yield under moderate conditions. The confined interface and optimized interfacial environment of the catalyst inside mesoporous silica contribute to the improved performance and stability.
ACS ES&T ENGINEERING
(2023)
Article
Multidisciplinary Sciences
Shenghui Zhou, Wenrui Ma, Uzma Anjum, Mohammadreza Kosari, Shibo Xi, Sergey M. Kozlov, Hua Chun Zeng
Summary: This study reports a mesoporous silica-encapsulated MoS2 catalyst with a fullerene-like structure and copper decoration for CO2 hydrogenation to methanol. The fullerene-like structure of MoS2 selectively exposes in-plane sulfur vacancies, while copper decoration promotes methanol yield and selectivity. Experimental and theoretical investigations confirm the critical role of strain in the catalytic reaction.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Tristan T. Y. Tan, Xin Li, Ken-ichi Otake, Ying Chuan Tan, Xian Jun Loh, Susumu Kitagawa, Jason Y. C. Lim
Summary: This study presents a direct method for synthesizing UiO-66 MOFs using adipic acid as a linker, which is traditionally overlooked. The research also demonstrates the feasibility of using adipic acid for MOF defect engineering.
CHEMICAL COMMUNICATIONS
(2022)