Article
Chemistry, Multidisciplinary
Somayeh Norouziyanlakvan, Gyandshwar Kumar Rao, Jeffrey Ovens, Bulat Gabidullin, Darrin Richeson
Summary: The study reports on the efficient electrocatalytic production of H-2 from mixed water/acetonitrile solutions using two new air-stable nickel(II) pincer complexes, demonstrating excellent Faradaic efficiency and turnover frequency. The catalysts may operate through a novel mechanism involving electron/proton transfer, displaying potential for reducing active proton sources at lower potentials.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Review
Chemistry, Multidisciplinary
Sebastian J. K. Forrest, Bastian Schluschass, Ekaterina Y. Yuzik-Klimova, Sven Schneider
Summary: The Haber-Bosch process, with its high carbon footprint, has sparked interest in alternative strategies for nitrogen fixation. Recent studies have shown that various metal compounds can effectively split N-2 at ambient conditions, offering potential for synthesizing nitrogen-containing products.
Article
Chemistry, Physical
Indranil Dutta, Nasser A. Alobaid, Fabio Lorenzo Menicucci, Priyanka Chakraborty, Chao Guan, Delong Han, Kuo-Wei Huang
Summary: The utilization of formic acid as a liquid organic hydrogen carrier has recently gained significant attention due to its desirable properties. In this study, a manganese complex [Mn(PN3P)(CO)2]Br was found to be an efficient catalyst for formic acid dehydrogenation, with a high turnover number (TON) of 15,200. This represents one of the best TON achieved using a manganese-based complex, demonstrating the importance of metal-ligand cooperativity in substrate activation for catalytic efficacy.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Applied
Yu Irie, Hongyu Chen, Hiromu Fuse, Harunobu Mitsunuma, Motomu Kanai
Summary: In this study, a linear-selective allylation reaction of aldehydes using simple alkenes as starting materials was developed by employing a quadruple hybrid catalyst system. The reaction proceeded under mild conditions, such as room temperature under visible light irradiation, and was applicable to asymmetric reactions. The addition of Ni(BF4)(2)center dot 6H(2)O catalyst to the previously reported ternary catalyst system accelerated the allylic transfer process from branch products to thermodynamically stable linear products by increasing the Bronsted acidity of thiophosphoric imide (TPI) catalyst.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Huatian Shi, Runhui Liang, David Lee Phillips, Hung Kay Lee, Wai-Lun Man, Kai-Chung Lau, Shek-Man Yiu, Tai-Chu Lau
Summary: In this study, a stable manganese(V) nitridocomplex was synthesized and its molecular structure and reactivity were investigated. The findings suggest that this complex exhibits high reactivity and can serve as a nitrene transfer reagent.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Biochemistry & Molecular Biology
Katja Bedbur, Nadja Stucke, Lina Liehrs, Jan Krahmer, Felix Tuczek
Summary: Three molybdenum trihalogenido complexes supported by different (PNP)-P-3 pincer ligands were synthesized and investigated for catalytic N-2-to-NH3 conversion. The H-(PNPtBu)-P-3 ligand showed the highest yields, and the corresponding Mo(V)-nitrido complex also exhibited good catalytic activity. Experiments on the formation of the analogous Mo(IV)-nitrido complex suggested that the catalytic mechanism of ammonia formation mediated by these systems follows the classic Chatt cycle, rather than N-N cleavage of a dinuclear Mo-dinitrogen complex.
Article
Chemistry, Multidisciplinary
Huatian Shi, Hung Kay Lee, Yi Pan, Kai-Chung Lau, Shek-Man Yiu, William W. Y. Lam, Wai-Lun Man, Tai-Chu Lau
Summary: This study presents the isolation and X-ray structure of a rare Mn(VI) nitrido complex, which exhibits N atom transfer reactions and catalytic abilities with NADH analogues.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Joel A. Rankin, Shramana Chatterjee, Zia Tariq, Satyanarayana Lagishetty, Benoit Desguin, Jian Hu, Robert P. Hausinger
Summary: Enzymes with the nickel-pincer nucleotide (NPN) cofactor catalyze C2 racemization or epimerization reactions of alpha-hydroxyacid substrates. LarB initiates synthesis of the NPN cofactor from nicotinic acid adenine dinucleotide (NaAD) by carboxylating the pyridinium ring C5 and hydrolyzing phosphoanhydride. LarB uses carbon dioxide as the substrate for carboxylation and activates water for hydrolytic attack on the C5-carboxylated-NaAD, enhancing reactivity. Structural studies show LarB has a unique N-terminal domain and a C-terminal domain homologous to PurE, with four active sites located at subunit interfaces. The complex of LarB with NAD* reveals a covalent adduct between Cys221 and NAD*, resulting in a boat-shaped dearomatized pyridine ring.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Multidisciplinary
Diego Martelino, Samyadeb Mahato, Warren VandeVen, Nicholas M. Hein, Ryan M. Clarke, Gregory A. MacNeil, Fabrice Thomas, Tim Storr
Summary: The oxidation location (metal or ligand) of Cr-V nitride salen complexes with different para-phenolate substituents was found to determine the reactivity of the nitride. One-electron oxidation results in Cr-VI nitrides and localized Cr-V nitride phenoxyl radicals, while oxidation to CrVI complexes leads to umpolung in reactivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Ji-Rui Li, Li-Ping Xu, Hui-Mei Jiang, Feng-Qin Wang, Jianhui Xie, Wai-Lun Man, Qian Wang, Shuping Zhuo, Tai-Chu Lau
Summary: The oxidation mechanism of hypophosphorous acid by a ruthenium(VI) nitrido complex was studied, revealing the dependence of reaction rate on the concentration of hypophosphorous acid and acidity. The rate-determining step involves the cleavage of the P-H bond. This study provides valuable insights into the kinetic properties of this reaction.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Han-Jun Ai, Yang Yuan, Xiao-Feng Wu
Summary: In this work, a pincer ruthenium-catalyzed heterocycle compatible alkoxycarbonylation of alkyl iodides has been developed, allowing efficient reaction with a variety of heterocyclic substrates.
Article
Chemistry, Multidisciplinary
Meghan J. Oddy, Daniel A. Kusza, Ryan G. Epton, Jason M. Lynam, William P. Unsworth, Wade F. Petersen
Summary: This study reports the synthesis of 2-azetidinones (beta-lactams) from simple acrylamide starting materials through visible-light-mediated energy transfer catalysis. The reaction involves a C(sp(3))-H functionalization via a variation of the Norrish-Yang photocyclization, which includes a carbon-to-carbon 1,5-hydrogen atom transfer. Deuterium labelling and DFT calculations support this mechanism, and the reaction can be used to construct a diverse range of beta-lactam products.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Amreen K. Bains, Yadav Ankit, Debashis Adhikari
Summary: This study reports a redox-active iminoquinone motif connected with a pi-delocalized pyrene core, capable of efficiently performing two-electron oxidation of a class of substrates. Inspired by the organic redox cofactor topaquinone (TPQ) in the enzyme copper amine oxidase, the molecule can easily oxidize primary and secondary alcohols in the presence of catalytic KOtBu. Under photoinduced conditions, the ligand backbone can be reduced to its iminosemiquinonate form, allowing for multi-component, one-pot coupling for the synthesis of quinoline and pyrimidine.
Article
Engineering, Environmental
Lele Zhao, Jiaming Zhang, Zhiping Zhang, Yujun Zhu, Yuan Zong, Chengying Bai, Tong Wei, Yueming Ren, Jun Ma
Summary: The effects of Cu oxidation states and reaction pH conditions on the properties of the copper-peroxy complex (---Cu-OOSO3-) and its catalytic degradation efficiency of bisphenol A were investigated. The results show that CuOx-30 with an average Cu valence of 1.61 exhibited the highest catalytic activity and electron-accepting ability. The reaction mechanism involved both single-electron transfer and oxygen-atom transfer pathways, which depended on the Cu oxidation states and reaction pH values.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Polymer Science
Yue-Fei Zhang, Jian Tang, Tao Li, Yun Liu, Yan Li
Summary: This paper reports the successful polymerization of acrolein via UV-mediated ATRP and identifies suitable experimental conditions. The polyacrolein synthesized can be potentially applied in fields such as biomedical labeling, immobilization carrier, and organic amine adsorption.
Article
Chemistry, Physical
Indranil Dutta, Nasser A. Alobaid, Fabio Lorenzo Menicucci, Priyanka Chakraborty, Chao Guan, Delong Han, Kuo-Wei Huang
Summary: The utilization of formic acid as a liquid organic hydrogen carrier has recently gained significant attention due to its desirable properties. In this study, a manganese complex [Mn(PN3P)(CO)2]Br was found to be an efficient catalyst for formic acid dehydrogenation, with a high turnover number (TON) of 15,200. This represents one of the best TON achieved using a manganese-based complex, demonstrating the importance of metal-ligand cooperativity in substrate activation for catalytic efficacy.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Multidisciplinary
Tamasgen Fikadu Yadeta, Kuo-Wei Huang, Toyoko Imae, Yung-Liang Tung
Summary: The high performance of perovskite solar cells was achieved by using an electron transport layer (ETL) and hole transport layer. A film ETL (mesoporous (meso)-TiO2/carbon dot) was found to enhance the efficiency of the perovskite solar cells. Coating carbon dot on a meso-TiO2 ETL was shown to reduce pin-holes in the perovskite film layer, resulting in a 3% increase in the average power conversion efficiency (PCE). The absorption properties of the meso-TiO2/carbon dot ETL were superior, leading to higher power conversion efficiency compared to meso-TiO2 ETL. The deposition of carbon dot on meso-TiO2 ETL reduced carrier recombination and perovskite film cracks, thereby improving device performance.
Article
Chemistry, Multidisciplinary
Areej Aljarb, Jiacheng Min, Mariam Hakami, Jui-Han Fu, Rehab Albaridy, Yi Wan, Sergei Lopatin, Dimitrios Kaltsas, Dipti Naphade, Emre Yengel, Mohamed Nejib Hedhili, Roaa Sait, Abdul-Hamid Emwas, Arwa Kutbee, Merfat Alsabban, Kuo-Wei Huang, Kaimin Shih, Leonidas Tsetseris, Thomas D. Anthopoulos, Vincent Tung, Lain-Jong Li
Summary: Growing continuous monolayer films of TMDs without disrupting grain boundaries is a challenge. The presence of an interfacial reconstructed (IR) layer within the substrate-epilayer gap affects the orientations of nucleating TMDs domains and materials' properties. These findings have implications for the development of TMD-based electronics and optoelectronics.
Article
Chemistry, Organic
Xinyu Liu, Zhixin Liu, Yongyi Hu, Kuo-Wei Huang, Manjaly J. Ajitha, De Wang
Summary: A novel alpha,beta-regioselective [3+2] cycloaddition reaction of arylallene with C,N-cyclic azomethine imine is reported. The axial-to-central chirality transfer phenomenon has been disclosed with chiral allenes in the reaction. The wide substrate scope, including different functional groups and natural products, reveals the generality of the methodology. Both experiments and density functional theory calculations have been used to elucidate a plausible mechanism.
Article
Chemistry, Multidisciplinary
Hao Huang, Dharmaraj Periyanagounder, Cailing Chen, Zhongxiao Li, Qiong Lei, Yu Han, Kuo-Wei Huang, Jr-Hau He
Summary: Developing a green and energy-saving artificial leaf for solar-driven ammonia conversion is achieved by imitating the biological nitrogen fixation and photosynthesis processes. The monolithic artificial leaf achieves high ammonia production rates and Faradaic efficiencies without applying external potential. By integrating an OER catalyst, the artificial leaf can directly convert solar energy into chemical energy and generate useful products. The importance rating of this research is 8 out of 10.
Article
Chemistry, Multidisciplinary
Tianyu Zheng, Rui Chen, Jingxian Huang, Theo P. Goncalves, Kuo-Wei Huang, Ying-Yeung Yeung
Summary: Bifunctional catalysis is important in synthesizing useful compounds. Confined bifunctional catalysts can achieve highly enantioselective reactions. This study demonstrates a proof-of-concept approach to formulating confined catalysts by linking catalytic species via non-covalent interactions. The reactions are optimized by changing the achiral catalyst.
Article
Engineering, Environmental
Hend Omar Mohamed, Vijay K. Velisoju, Idoia Hita, Omar Abed, Rajesh K. Parsapur, Naydu Zambrano, Mohamed Ben Hassine, Natalia Morlanes, Abdul-Hamid Emwas, Kuo-Wei Huang, Pedro Castano
Summary: By using the in situ modified zeolite technique, researchers have successfully developed an efficient catalyst with high Ni2+ species concentration and good dispersion, which can improve the yield and stability of 1-butene while reducing the formation of by-products.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Fatimah Mohammad H. Al Sulami, Merfat M. Alsabban, Ahlam I. Al-Sulami, Mohamed Farrag, Sylvain Vedraine, Kuo-Wei Huang, Eslam Sheha, Talaat A. Hameed
Summary: Replacing selenium with sulfur in Cu1.8Se can improve the low electronic conductivity of Cu-Se and mitigate the effect of polysulfide species. A Cu1.8Se0.6S0.4 nanocrystalline powder was synthesized by solid-state reaction and its structure and storage mechanism were confirmed by various characterization techniques. Significant surface morphology changes were observed during the charging/discharging process.
Article
Chemistry, Physical
Xingzhu Chen, Luigi Cavallo, Kuo-Wei Huang
Summary: In the past decade, density functional theory (DFT) calculations have been used to investigate the mechanism of electrochemical CO2 reduction reactions. However, the lack of understanding regarding CO2 chemisorption states, proton-coupled-electron-transfer (PCET) steps, and dynamic redox reactions of the electrode surface has limited the reliability of these simulations. This work proposes a descriptor, the energy difference between *COOH on neutral and extra-electron substrates, as a means to determine the selectivity of electrochemical CO2 reduction.
Article
Chemistry, Organic
Delong Han, Priyanka Chakraborty, Li Yang, Hao Huang, Kuo-Wei Huang
Summary: Alkylation of a nitride ligand of a post-modified Mo(V) complex with MeOTf and EtOTf resulted in the formation of highly stable Mo(IV) imido complexes. Unlike the known Mo(VI) nitride complexes, which can be deprotonated to form ketimide for further reactions, the alkylation products in this study could only be reduced by NaH. Treatment with PhCH2OTf led to the formation of a new dinuclear Mo complex with N-2 release, instead of benzylation of the nitride ligand.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Chen-Fu Lin, Kuo-Wei Huang, Yen-Ting Chen, Sung-Lin Hsueh, Ming-Hsien Li, Peter Chen
Summary: This review introduces X-ray detectors using various halide perovskite materials and discusses their performance. Single-crystal perovskite as an active material exhibits excellent performance under X-ray illumination, while inorganic perovskite shows good environmental stability and high X-ray sensitivity. Double perovskite with the introduction of high-atomic-numbered elements demonstrates better attenuation of X-rays, and lead-free perovskite exhibits potential application in X-ray detectors due to its high X-ray attenuation capability. The up-scaling process technology for fabricating large-area and thick perovskite films for X-ray detectors is also introduced.
Editorial Material
Chemistry, Physical
Indranil Dutta, Rajesh Kumar Parsapur, Sudipta Chatterjee, Amol M. Hengne, Davin Tan, Karthik Peramaiah, Theis I. Solling, Ole John Nielsen, Kuo-Wei Huang
ACS ENERGY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Jian-Xin Wang, Indranil Dutta, Jun Yin, Tengyue He, Luis Gutierrez-Arzaluz, Osman M. Bakr, Mohamed Eddaoudi, Kuo-Wei Huang, Omar F. Mohammed
Summary: In this study, a highly efficient and reabsorption-free transparent X-ray imaging scintillator was fabricated by utilizing an efficient triplet-triplet energy transfer strategy between TADF-Br and Ir-OMC. The experiments and calculations showed that efficient energy transfer from TADF-Br to Ir-OMC can be achieved, leading to enhanced triplet-state radioluminescence upon X-ray irradiation. The fabricated scintillator achieved a high X-ray imaging resolution of 19.8 lp mm -1 .
Review
Chemistry, Multidisciplinary
Bin Chang, Hong Pang, Fazal Raziq, Sibo Wang, Kuo-Wei Huang, Jinhua Ye, Huabin Zhang
Summary: In this review, the recent progress and challenges in preparing C2+ products are discussed. The recent advancements in carbon-carbon coupling results and proposed mechanisms are elaborated, along with the complex scenarios involved in the initial CO2 activation process, catalyst micro/nanostructure design, and mass transfer conditions optimization. The synergistic realization of high C2+ product selectivity through catalyst design and the influence of electrolytes using theoretical calculation analysis and machine learning prediction are also proposed. The in situ/operando techniques for tracking structural evolution and recording reaction intermediates during electrocatalysis are elaborated, as well as insights into triphasic interfacial reaction systems with improved C2+ selectivity.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Lujain Alrais, Sandeep Suryabhan Gholap, Indranil Dutta, Edy Abou-Hamad, Benjamin W. J. Chen, Jia Zhang, Mohamed Nejib Hedhili, Jean-Marie Basset, Kuo-Wei Huang
Summary: Formic acid is a promising hydrogen carrier for on-demand hydrogen generation. By immobilizing a homogeneous PN3P-Ir pincer catalyst onto a support, the advantages of both homogeneous and heterogeneous catalysts can be combined. The use of cesium formate as a reaction medium and basic additive under suitable conditions significantly improves the reactivity.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Review
Chemistry, Multidisciplinary
Dan He, Yawen Li, Fuwen Zhao, Yuze Lin
Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.
CHEMICAL COMMUNICATIONS
(2024)
Review
Chemistry, Multidisciplinary
Olivier Monfort, Arshitha Madhusudhan, Martin Motola
Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna
Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi
Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang
Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell
Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini
Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar
Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan
Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal
Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi
Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.
CHEMICAL COMMUNICATIONS
(2024)
