Article
Chemistry, Multidisciplinary
Z. Tian, C. Dong, D. Li, G. -H. Wang
Summary: The highly selective semihydrogenation of alkynes can be achieved using bimetallic palladium catalysts in a two-chamber reactor, efficiently utilizing H-2 and selectively producing alkenes under mild reaction conditions. The Pd-based bimetallic catalysts show excellent catalytic performances for semihydrogenation of alkynes and dehydrogenation of formic acid in the two-chamber reactor.
MATERIALS TODAY CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Naoki Ishida, Yoshiki Kamae, Keigo Ishizu, Yuka Kamino, Hiroshi Naruse, Masahiro Murakami
Summary: The system described in the passage utilizes solar energy to capture, store, and release chemical energy for hydrogenation. Through a two-step process, solar energy is converted into chemical energy, which is then used for hydrogenation, with the advantage of easy recovery and reuse.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Alejandro Valiente, Pablo Martinez-Pardo, Gurpreet Kaur, Magnus J. Johansson, Belen Martin-Matute
Summary: This paper presents a method for the electrochemical semihydrogenation and semideuteration of alkynes to form Z-alkenes using nickel foam as a catalyst. The reaction demonstrated good yields and excellent stereoselectivities under mild conditions, showing versatility in substrates. The recyclability of the nickel foam electrocatalyst was up to 14 cycles without loss of catalytic properties.
Article
Chemistry, Physical
Ke Chen, Hongdan Zhu, Yuling Li, Qian Peng, Yinlong Guo, Xiaoming Wang
Summary: The switchable semireduction of alkynes to (Z)- or (E)-alkenes catalyzed by a dinuclear cobalt complex supported by a macrocyclic bis pyridyl diimine (PDI) ligand allows control of the stereoisomerization process by adjusting the amount of water, providing a convenient method for obtaining either (Z)- or (E)-olefin isomer in a single transformation.
Article
Chemistry, Physical
Kaili Zhu, Jun Ma, Liang Chen, Fangfang Wu, Xudong Xu, Mengqiu Xu, Wei Ye, Yao Wang, Peng Gao, Yujie Xiong
Summary: By designing the catalyst based on the interfacial water structure, this study achieved high activity and selectivity in electrochemical semihydrogenation. Experimental results showed that PdFe nanosheets could continuously produce a large amount of alkynes for 264 hours, demonstrating significant advantages over traditional thermal semihydrogenation methods in terms of performance, energy, and cost.
Article
Chemistry, Physical
Heiko Schratzberger, Berthold Stoeger, Luis F. Veiros, Karl Kirchner
Summary: In this study, two stable Fe(II) alkyl complexes were successfully synthesized and their catalytic performance in transfer hydrogenation reactions was investigated. The results showed that these complexes exhibited good activity and selectivity for hydrogenation of various alkynes. Through both experimental and theoretical investigations, the researchers also revealed the reaction mechanism.
Article
Chemistry, Physical
Ronald A. Farrar-Tobar, Stefan Weber, Zita Csendes, Antonio Ammaturo, Sarah Fleissner, Helmuth Hoffmann, Luis F. Veiros, Karl Kirchner
Summary: This study describes the selective semihydrogenation of alkynes using a Mn(I) alkyl catalyst, leading to good to excellent yields of E-alkenes. Mechanistic investigations reveal that the initially formed Z-isomer undergoes fast isomerization to the thermodynamically more stable E-isomer.
Article
Chemistry, Physical
Tsuyoshi Yamada, Haruka Yamamoto, Kanon Kawai, Kwihwan Park, Norihiko Aono, Hironao Sajiki
Summary: Silicon carbide-supported palladium catalyst has been developed for selective hydrogenation reactions, showing excellent selectivity and tolerance to various functional groups. The combination of DETA with the catalyst demonstrated higher chemoselectivity in continuous-flow conditions.
Article
Chemistry, Multidisciplinary
Han-Ying Liu, Samuel E. Neale, Michael S. Hill, Mary F. Mahon, Claire L. McMullin
Summary: The copper(i) alumanyl derivative reacts with up to three equivalents of various terminal alkynes, resulting in the sequential formation of cuprous (hydrido)(alkynyl)aluminate, (alkenyl)(alkynyl)aluminate, and bis(alkynyl)aluminate derivatives. The alkene liberation process in the latter step is a unique case of alkyne transfer semi-hydrogenation.
Article
Chemistry, Multidisciplinary
Minda Chen, Geet Gupta, Claudio W. Ordonez, Andrew R. Lamkins, Charles J. Ward, Celia A. Abolafia, Biying Zhang, Luke T. Roling, Wenyu Huang
Summary: RhZn intermetallic nanoparticles have been developed as an exceptional catalyst for efficient heterogeneous hydroformylation, showing high activity and selectivity compared to traditional homogeneous catalysts. Density functional theory calculations reveal that RhZn surfaces reduce the binding strength of reaction intermediates and have lower activation energy barriers, leading to more favorable reaction energetics. Additionally, potential catalyst design strategies for achieving high regioselectivity have been predicted.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Rui Zhang, Zhilin Liu, Shaohang Zheng, Luoqi Wang, Ling Zhang, Zhen-An Qiao
Summary: Supported metal catalysts, especially nitrogen-doped carbon support materials, have been extensively studied for optimizing the selective semihydrogenation of alkynes. It remains a challenge to identify the dominant nitrogen configuration that affects the catalytic behavior. In this study, uniform mesoporous N-doped carbon spheres were used as supports to immobilize subnanometric Pd clusters, revealing that pyridinic nitrogen configuration plays a crucial role in enhancing catalytic activity and selectivity. The presence of abundant coordination sites and the electron effect between pyridinic nitrogen sites and Pd clusters contribute to the improved catalytic performance.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Matteo Vanni, Marco Bellini, Silvia Borsacchi, Lucia Calucci, Maria Caporali, Stefano Caporali, Francesco d'Acapito, Marco Geppi, Andrea Giaccherini, Andrea Ienco, Gabriele Manca, Antonio Massimiliano Mio, Giuseppe Nicotra, Werner Oberhauser, Manuel Serrano-Ruiz, Martina Banchelli, Francesco Vizza, Maurizio Peruzzini
Summary: This study provides the first complete structural characterization of 2D BP functionalized with rare discrete Pd-2 units, revealing the existence of interlayer Pd-Pd units and an increase in catalytic activity for the hydrogen evolution reaction. Multiple techniques were utilized to study the morphology of Pd-2/BP nanosheets and to uncover the coordination of Pd-2 units to phosphorus atoms in 2D BP. The presence of Pd-2 units was found to enhance the activity of Pd-2/BP as a catalyst for HER in acidic medium.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Karim Azouzi, Dmitry A. Valyaev, Stephanie Bastin, Jean-Baptiste Sortais
Summary: This review comprehensively covers transfer hydrogenation processes catalyzed by manganese organometallic complexes, with a focus on reduction reactions of various substances and ligand design for Mn-catalyzed asymmetric transfer hydrogenation reactions.
CURRENT OPINION IN GREEN AND SUSTAINABLE CHEMISTRY
(2021)
Article
Chemistry, Physical
Lei Wang, Peng Yin, Wei-Jie Zeng, Shi-Long Xu, Ping Chen, Hai-Wei Liang
Summary: The synthesis of small-sized Pd3Pb intermetallic nanocatalysts with improved catalytic performance is achieved by using a bulky nanodiamond-confined method. The resulting catalyst exhibits high activity and selectivity under mild conditions.
Article
Multidisciplinary Sciences
Shuang Liu, Yong Li, Xiaojuan Yu, Shaobo Han, Yan Zhou, Yuqi Yang, Hao Zhang, Zheng Jiang, Chuwei Zhu, Wei-Xue Li, Christof Woll, Yuemin Wang, Wenjie Shen
Summary: Bimetallic nanoparticles with geometric variation and electron redistribution can greatly enhance catalytic activity and selectivity. However, quantitatively describing the atomic configuration of catalytically active sites is challenging due to the interplay between particle size and crystal phase. In this study, the authors demonstrate that tuning the crystal phase of metal single-particles allows for accurate description of the atomic structure of active sites.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yu Tian, Yuling Zhao, Fanqi Meng, Kaicheng Zhang, Yanyuan Qi, Yujie Zeng, Congcong Cai, Yuli Xiong, Zelang Jian, Yang Sun, Lin Gu, Wen Chen
Summary: Substituting Mn and Li in the Mn/Li transition metal layer with Ti can stabilize the structure of Li2MnO3 and promote Li-ion diffusion. This strategy also increases the capacity and cycling performance of lithium-rich layered oxide cathodes for lithium-ion batteries.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Qiao Jin, Qinghua Zhang, He Bai, Amanda Huon, Timothy Charlton, Shengru Chen, Shan Lin, Haitao Hong, Ting Cui, Can Wang, Haizhong Guo, Lin Gu, Tao Zhu, Michael R. Fitzsimmons, Kui-juan Jin, Shanmin Wang, Er-Jia Guo
Summary: By synthesizing single-crystalline and precisely controlled Fe3N thin films, this study demonstrates the maintenance of high-temperature ferromagnetism in thin Fe3N layers and reveals strong in-plane anisotropy and changing anomalous Hall resistivity. Additionally, a significant exchange bias is observed at the Fe3N and CrN interfaces. This work provides guidance for exploring functional nitride films and their potential applications.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Shengru Chen, Qinghua Zhang, Dongke Rong, Yue Xu, Jinfeng Zhang, Fangfang Pei, He Bai, Yan-Xing Shang, Shan Lin, Qiao Jin, Haitao Hong, Can Wang, Wensheng Yan, Haizhong Guo, Tao Zhu, Lin Gu, Yu Gong, Qian Li, Lingfei Wang, Gang-Qin Liu, Kui-juan Jin, Er-Jia Guo
Summary: This study reports the creation of morphotropic grain boundaries in laterally interconnected cobaltite homostructures. By modulating and isolating electronic states and magnetic behavior through the grain boundaries, artificially engineered functionalities can be achieved in the planar matrix.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zhexin Tang, Tongtong Shang, Han Xu, Ting Lin, Ang Gao, Weiguang Lin, Xinyan Li, Shiyu Wang, Botao Yu, Fanqi Meng, Qinghua Zhang, Xuefeng Wang, Dong Su, Qingbo Meng, Lijun Wu, Lin Gu, Ce-Wen Nan
Summary: The physical properties of materials are determined by the valence electron configurations, and different valence shells lead to different phenomena. In this study, we examined the valence electron density and orbital population of Sc2+ in the compound ScS using quantitative convergent-beam electron diffraction. Our results show that the 4s orbital is occupied by Sc2+, which is unexpected as it is usually the 3d orbital that is occupied in transition metal atoms. This finding reveals a unique electron configuration in a transition metal compound and suggests potential ways to modulate material properties by controlling electron orbitals.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Zhi-Mo Zhang, Ben-Chao Gong, Jin-Hua Nie, Fanqi Meng, Qinghua Zhang, Lin Gu, Kai Liu, Zhong-Yi Lu, Ying-Shuang Fu, Wenhao Zhang
Summary: By self-intercalating Fe atoms into the van der Waals gap of FeSe2 using molecular beam epitaxy, we successfully constructed kagome-like structures. The resulting Fe5Se8 stoichiometry was observed using low-temperature scanning tunneling microscopy, showing the emergence of a 2 x 2 ordered Fe atom arrangement. The kagome pattern mainly originates from the slight reconstruction of topmost Se atoms due to the non-equivalent subsurface Fe sites caused by intercalation. This study presents an alternative approach for constructing artificial kagome structures, opening up possibilities for exploring correlated quantum states.
Article
Chemistry, Multidisciplinary
Kai Wang, Jinhui Zhou, Mingzi Sun, Fangxu Lin, Bolong Huang, Fan Lv, Lingyou Zeng, Qinghua Zhang, Lin Gu, Mingchuan Luo, Shaojun Guo
Summary: We report a new design of Cu-doped Ru/RuSe2 heterogeneous nanosheets (NSs) with optimized H and H2O adsorption strength for highly efficient HER catalysis in alkaline media. The Cu-doped Ru/RuSe2 NSs exhibit a small overpotential, low Tafel slope, and high turnover frequency for HER, making them among the best catalysts in noble metal-based electrocatalysts toward HER. This work demonstrates that heterogeneous interface modulation opens up a new strategy for the designing of more efficient electrocatalysts.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Tingting Hu, Weicheng Shen, Fanqi Meng, Shuqing Yang, Shilong Yu, Hai Li, Qinghua Zhang, Lin Gu, Chaoliang Tan, Ruizheng Liang
Summary: Sonodynamic therapy (SDT) has shown promise as a cancer treatment, and researchers have developed ultrathin nanosheets as highly efficient sonosensitizers for SDT. The nanosheets undergo a phase transformation from polycrystalline to amorphous, resulting in higher reactive oxygen species (ROS) generation activity under ultrasound (US) irradiation. The enhanced performance of the nanosheets can be attributed to defect generation and electronic structure changes caused by the phase transformation. With polyethylene glycol modification, the nanosheets can effectively induce cell death in vitro and tumor eradication in vivo under US irradiation.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Xinyan Li, Hai Zhong, Ting Lin, Fanqi Meng, Ang Gao, Zhuohui Liu, Dong Su, Kuijuan Jin, Chen Ge, Qinghua Zhang, Lin Gu
Summary: In this work, the researchers used low-dose integrated differential phase-contrast scanning transmission electron microscopy (iDPC-STEM) to directly observe the oxygen shifting and polar-nonpolar phase transitions in freestanding ZrO2 thin films. They clarified bidirectional transitions between antiferroelectric and ferroelectric orders and explained the mechanism of interfacial polarization relaxation at the unit-cell scale. The polarization switching was found to be strongly correlated with Zr-O displacement and two-step tetrahedral-to-orthorhombic phase transition.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Ruyi Zhang, Ting Lin, Shaoqin Peng, Jiachang Bi, Shunda Zhang, Guanhua Su, Jie Sun, Junhua Gao, Hongtao Cao, Qinghua Zhang, Lin Gu, Yanwei Cao
Summary: Flexible single-crystalline plasmonic or photonic components are synthesized by depositing refractory nitride superlattices on flexible fluorophlogopite-mica substrates. These flexible materials exhibit dual-band hyperbolic dispersion of dielectric constants with low dielectric losses and high figures of merit in the visible to near-infrared ranges. The optical properties of these nitride-based materials remain stable even after exposure to high temperature or repeated bending, making them ideal for flexible electronic and photonic devices.
Article
Chemistry, Physical
Yanan Xu, Kai Wang, Xudong Zhang, Yibo Ma, Qifan Peng, Yue Gong, Sha Yi, Hua Guo, Xiong Zhang, Xianzhong Sun, Hongcai Gao, Sen Xin, Yu-Guo Guo, Yanwei Ma
Summary: A 10-nm polydopamine coating on the residue-removed garnet surface is shown to stabilize the modified garnet filler and prevent the generation of alkaline residues, allowing PVDF to remain intact. Metal-nitrogen bonding between the La atoms of garnet and the amino groups of polydopamine promotes stronger adsorption of Li ions, enabling an efficient ion-percolation network for Li-ion conduction through the garnet-polydopamine interface. The composite electrolyte demonstrates an effective room-temperature Li+ conductivity of 1.52 x 10(-4) S cm(-1) and a high cutoff voltage of up to 4.7 V versus Li+/Li to support stable operation of all-solid-state Li-LiCoO2 batteries.
ADVANCED ENERGY MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Shuai Liu, Xuwei Cui, Qinghua Zhang, Wanfu Shen, JianTao Du, Ting Lin, Yunkun Wang, Minghui Wu, Lin Gu, Yunan Gao, Chunguang Hu, Luqi Liu, Shengxue Yang, Chengbao Jiang
Summary: This study reports on an interesting low-symmetry 2D material, GaPS4, and investigates its in-plane anisotropic structure, optical, and mechanical properties. The experimental results show that GaPS4 is sensitive to crystalline orientation and linear dichroism. An interesting pressurized bubble method is used to verify the anisotropic mechanical properties of GaPS4, and saddle-like bubble devices of GaPS4 are successfully fabricated.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Multidisciplinary Sciences
Yunhao Wang, Mingzi Sun, Jingwen Zhou, Yuecheng Xiong, Qinghua Zhang, Chenliang Ye, Xixi Wang, Pengyi Lu, Tianyi Feng, Fengkun Hao, Fu Liu, Juan Wang, Yangbo Ma, Jinwen Yin, Shengqi Chu, Lin Gu, Bolong Huang, Zhanxi Fan
Summary: This study presents the one pot synthesis of ultrathin nanosheet-assembled RuFe nanoflowers with low-coordinated Ru sites for enhanced electrochemical nitrate reduction reaction (NO3RR). The RuFe nanoflowers exhibit high ammonia FE and yield rate in neutral electrolyte, thanks to their highly electroactive nature and efficient electron transfer. The demonstration of rechargeable zinc-nitrate batteries further highlights the great potential of RuFe nanoflowers in next-generation electrochemical energy systems.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Physical
Xincheng Lei, Yingying Wang, Jiayi Wang, Yi Su, Pengxiang Ji, Xiaozhi Liu, Shengnan Guo, Xuefeng Wang, Qingmiao Hu, Lin Gu, Yuegang Zhang, Rui Yang, Gang Zhou, Dong Su
Summary: Despite its high energy density, only a small portion of silicon has been utilized as an anode material in commercial lithium-ion batteries. This study proposes a Si-based high-entropy alloy (HEA) material as an alternative anode material, which shows high structural stability. The incorporation of HEA elements in the Si anode decreases anisotropic stress and enhances ductility, resulting in improved cycling stability. The reversible lithiation and delithiation process between HEA phases contribute to the intrinsic stability. The findings suggest that incorporating high-entropy modification is a promising approach in designing anode materials for high-energy density LIBs.
Article
Materials Science, Multidisciplinary
Zhaoqing Ding, Xuejiao Chen, Zhenzhen Wang, Qinghua Zhang, Fang Yang, Jiachang Bi, Ting Lin, Zhen Wang, Xiaofeng Wu, Minghui Gu, Meng Meng, Yanwei Cao, Lin Gu, Jiandi Zhang, Zhicheng Zhong, Xiaoran Liu, Jiandong Guo
Summary: This research establishes an emergent trigonal structure of SrRuO3 through heteroepitaxial strain engineering along the [111] crystallographic axis. The trigonal SrRuO3 exhibits a peculiar XY-type ferromagnetic ground state and the coexistence of high-mobility holes from linear Weyl bands and low-mobility electrons from normal quadratic bands as carriers. Experimental observations are consistent with first-principles calculations, shedding light on the detailed band topology of trigonal SrRuO3 with multiple pairs of Weyl nodes near the Fermi level. This study signifies the potential of lattice design in manipulating magnetism and Berry phase, and unveils nontrivial correlated topological phenomena.
NPJ QUANTUM MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Changchun Ye, Zhenghui Pan, Qinghua Zhang, Fang Yin, Yanan Wang, Yifei Li, Guangxu Chen, Jia Li, Yongcai Qiu, Geoffrey I. N. Waterhouse, Lin Gu, Zhang Lin, Lin Guo
Summary: A facile synthesis route for heterostructured metal oxides via quenching-induced structural transformation was developed. Multiple quenching triggered the transformation from NiMoO4 to NiFe2O4, creating a novel heterostructure, and the pre-quenching generated disordered defect structure can promote subsequent quenching regulation.
ENERGY & ENVIRONMENTAL SCIENCE
(2024)