Article
Chemistry, Multidisciplinary
Menglei Yuan, Junwu Chen, Yong Xu, Rongji Liu, Tongkun Zhao, Jingxian Zhang, Zhongyu Ren, Zhanjun Liu, Carsten Streb, Hongyan He, Chao Yang, Suojiang Zhang, Guangjin Zhang
Summary: The study achieved efficient conversion of CO2 and N-2 into urea by precisely designing unique frustrated Lewis pairs in flower-like nickel borate crystals. Through the synergistic action of Lewis acidic and basic sites, inert gases were captured and activated, ultimately achieving high urea yield rates.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Physical
P. Konik, E. Berdonosova, I. Savvotin, V. Zadorozhnyy, M. Zadorozhnyy, D. Semenov, A. Korol, A. Kvaratskheliya, S. Klyamkin
Summary: Short-term mechanical activation in a ball mill can significantly change the pressure-composition isotherms, lattice strain, and coherent scattering domain size of alloys, while reducing the volume expansion of certain alloy lattices. The study shows that mechanically activated alloys have different application potentials, allowing for the selection of appropriate materials based on various pressure and temperature requirements.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Inorganic & Nuclear
Steven M. Rehbein, Matthew J. Kania, Sharon R. Neufeldt
Summary: Research indicates that tantalocene hydrides can catalyze H/D exchange with arenes, with a mechanism involving oxidative addition at transient T-III. The reaction with benzene-d6 was found to be moderately faster under thermal conditions compared to photochemical conditions. Cp2TaH3 activates aromatic C-(sp2)-H bonds during the reaction, but not benzylic bonds.
Article
Materials Science, Multidisciplinary
Vasil M. Garamus, Wolfgang Limberg, Maria Serdechnova, Di Mei, Sviatlana Lamaka, Thomas Ebel, Regine Willumeit-Roemer
Summary: Multifunctional materials based on a combination of permanent and degradable metals were investigated for medical implants with osseoconductivity and drug-delivery functions. The study showed that controlling the degradation of the magnesium part and modifying the titanium part were necessary for developing partly degradable hybrid implants.
Article
Chemistry, Physical
Huang Liu, Jingxi Zhang, Pei Sun, Chengshang Zhou, Yong Liu, Zhigang Zak Fang
Summary: TiFe alloy is an excellent candidate for stationary hydrogen storage due to its superior properties. However, the need for high-temperature activation has hindered its practical application. This study investigates the activation of TiFe alloys with different ratios and finds that TiFe0.90 alloy can be activated at room temperature and moderate hydrogen pressure, while equimolar TiFe alloy has poor activation kinetics. The presence of Ti4Fe2O1-x phase in the TiFe0.9 alloy plays a critical role in the activation process, serving as a conduit for hydrogen absorption by TiFe.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Engineering, Environmental
Zhuanghe Ren, Xin Zhang, Zhenguo Huang, Jianjiang Hu, Yangzhong Li, Shiyou Zheng, Mingxia Gao, Hongge Pan, Yongfeng Liu
Summary: Nanosized TiH2 flakes were successfully synthesized through a one-pot solvothermal process and epitaxially grown on graphene surface. The generation of Cl· radicals and unsaturated C=C bonds during the reaction of TiCl4 with THF promoted the formation of TiH2. The nanoflake-like TiH2 enabled outstanding hydrogen storage performance of NaAlH4.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Qing Tan, Zhiran Yan, Runguang Li, Yang Ren, Yandong Wang, Baptiste Gault, Stoichko Antonov
Summary: This study investigates the deformation behavior of hydrogen-charged commercially pure titanium using in-situ high energy X-ray diffraction. The results reveal that the peak broadening in the diffusion patterns is caused by high internal and interphase stresses generated within and around the hydrides due to volume expansion caused by phase transformation. The hydrides exhibit high strength but brittle secondary phase behavior and sustain larger strains than the matrix. This study provides valuable insights into hydride deformation behavior and hydrogen embrittlement in titanium and zirconium.
SCRIPTA MATERIALIA
(2022)
Article
Chemistry, Multidisciplinary
Gao-Xiang Wang, Xuechao Yan, Jianhao Yin, Zhu-Bao Yin, Junnian Wei, Zhenfeng Xi
Summary: A series of novel cobalt complexes were successfully synthesized in this study, and their structures and reactivity were confirmed through experiments and DFT calculations.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Yuanyuan Shang, Claudio Pistidda, Chiara Milanese, Alessandro Girella, Alexander Schokel, Thi Thu Le, Annbritt Hagenah, Oliver Metz, Thomas Klassen, Martin Dornheim
Summary: This manuscript proposes a method for obtaining high-quality NaAlH4 from automotive recycled alloy, and comprehensively explores its hydrogen storage properties using various experimental techniques. The results show that NaAlH4 with comparable properties to high-purity commercial NaAlH4 was successfully synthesized.
Article
Chemistry, Physical
Hongying Li, Bicheng Zhu, Jian Sun, Haiming Gong, Jiaguo Yu, Liuyang Zhang
Summary: Compared to hydrogen production through pure water photocatalysis, utilizing seawater directly for hydrogen production is more in line with the principles of sustainable development. RuO2 and TiO2 have been widely recognized to exhibit good stability in seawater. This study investigates hydrogen production in simulated seawater using a RuO2-modified TiO2 model system. The results show that the hydrogen production activity of TiO2/RuO2 nanofibers in simulated seawater is comparable to that in pure water.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2024)
Article
Chemistry, Applied
Clement Maheu, Eric Puzenat, Pavel Afanasiev, Luis Cardenas, Christophe Geantet
Summary: This study investigated the influence of seven parameters on the photocatalytic production of hydrogen, including the optimal electron transfer from TiO2 to RuS2 at the rate-determining step. The photon yield showed an optimum at specific co-catalyst loading level, demonstrating the potential for optimizing electron transfer with incident photons having higher energy levels.
Article
Chemistry, Physical
Huang Liu, Jingxi Zhang, Chengshang Zhou, Pei Sun, Yong Liu, Zhigang Zak Fang
Summary: This paper investigates the effect of Nb alloying on the microstructure and hydrogen storage properties of Ti-Fe-Zr-Mn-Nbx alloys. The addition of 2% Nb enables a good combination of the hydrogen capacity and activation property, while Zr-rich phases play a critical role in the activation behavior. However, high Nb addition (> 4%) leads to the reduction of Zr-rich phases and deteriorates the activation kinetics. Nb addition also promotes the formation of the TiFe main phase and increases capacities at ambient temperature. The correlations between microstructure and hydrogen storage performance provide insights into tailoring hydrogen storage properties by alloying TiFe with multi-elements.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Physical
Shashi Sharma, Rini Singh, Takayuki Ichikawa, Ankur Jain, Shivani Agarwal
Summary: Hydrogen as an energy carrier has great potential for future energy infrastructure. The storage of hydrogen in solid state materials, such as KSiH3, has been proposed as a safe method. In this study, vanadium-based catalysts, particularly V2O5, were added to enhance the kinetics and reduce the activation energy of the KSiH3 system. The addition of V2O5 catalyst enabled hydrogen desorption at lower temperatures and achieved a high weight loss close to the theoretical value, indicating improved reversibility and hydrogen storage capacity.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Physical
David Michael Dreistadt, Le Thi-Thu, Giovanni Capurso, Jose M. Bellosta von Colbe, Archa Santhosh, Claudio Pistidda, Nico Scharnagl, Henry Ovri, Chiara Milanese, Paul Jerabek, Thomas Klassen, Julian Jepsen
Summary: This work proposes an effective thermal activation method for industrially produced titanium-iron-manganese powders for hydrogen storage. It is found that lower temperatures and larger particle sizes lead to better activation performance. The proposed method overcomes the diffusion barrier of the oxide layer, resulting in faster sorption kinetics.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Review
Chemistry, Inorganic & Nuclear
Takanori Shima, Qingde Zhuo, Zhaomin Hou
Summary: This review summarizes the recent progress in N2 activation and transformation by molecular multimetallic polyhydride complexes. These complexes exhibit unique activity and selectivity, allowing for N2 cleavage and hydrogenation without the need for special reductants or proton sources. The activated nitrogen species in a multimetallic framework can react with various electrophiles, leading to the formation of new chemical bonds.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Xuefeng Cong, Qingde Zhuo, Na Hao, Zhenbo Mo, Gu Zhan, Masayoshi Nishiura, Zhaomin Hou
Summary: This study presents the regio- and diastereoselective [3+2] annulation of aliphatic aldimines with alkenes using half-sandwich scandium catalysts, providing a new family of multi-substituted aminocyclopentane derivatives. Styrenes reacted exclusively to afford 5-aryl-trans-substituted 1-aminocyclopentane derivatives with excellent diastereoselectivity, while aliphatic alkenes selectively gave 4-alkyl-trans-substituted 1-aminocyclopentane products. The addition of a catalytic amount of appropriate amines significantly influenced catalyst activity and stereoselectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Jimin Yang, Qingde Zhuo, Zhenbo Mo, Zhaomin Hou, Yi Luo
Summary: The mechanism of dinitrogen cleavage by a PNP-coordinated dititanium polyhydride complex has been computationally investigated, revealing a multi-state reactivity scenario for the process. Prior to N-N cleavage, H-2 elimination is facilitated by coupling two terminal hydrides, with stabilization provided by a planar PNP-pincer ligand. Additionally, the THF solvent promotes H-2 elimination due to the similar polarity of intermediates or transition states.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Gang Xiong, Olivier Tardif, Masayoshi Nishiura, Guan Bingtao, Zhaomin Hou
Summary: The synthesis and transformation of a new family of half-sandwich dialkynyl complexes have been reported, showing diverse structural features depending on metal ion size, alkyne substituent, and presence of THF coordination. Acid-base reactions between half-sandwich rare earth dialkyl complexes and terminal alkynes generally produced monomeric rare earth dialkynyl complexes with THF coordination, which could further aggregate upon recrystallization.
HELVETICA CHIMICA ACTA
(2022)
Article
Chemistry, Multidisciplinary
Qingde Zhuo, Jimin Yang, Zhenbo Mo, Xiaoxi Zhou, Takanori Shima, Yi Luo, Zhaomin Hou
Summary: The reaction of N2 with CO2 in a dititanium dihydride framework has been reported for the first time, resulting in N-C bond formation and cleavage of N-N and C-O bonds. The selectivity of the reaction products was found to be influenced by temperature. Mechanistic details were clarified through isotope-labeling experiments.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Lei Jiang, Yinran Wang, Hanyang Sun, Tingting Fu, Zhaomin Hou, Fang Guo
Summary: This study successfully achieved the coordination polymerization of diphenylphosphinostyrene and its copolymerization with styrene, resulting in a new series of phosphine functionalized syndiotactic polystyrene with excellent thermal stability and chemical resistance. The combination of triphenylphosphine and syndiotactic polystyrene allowed for the stable immobilization of metal nanoparticles to form highly robust nanocatalysts, showing high efficiency as a heterogeneous catalyst for the synthesis of quinoline derivatives.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Polymer Science
Fen You, Xiaohui Kang, Masayoshi Nishiura, Jingjing Zhai, Suting Xu, Jixing Wang, Xiaochao Shi, Zhaomin Hou
Summary: This study reports the living and highly 3,4-isoselective polymerization of biobased monomer beta-farnesene using a phosphine-functionalized fluorenyl-ligated yttrium catalytic system. The coordination of the phosphine group plays a pivotal role in the regio- and stereoselectivity of the polymerization. Block copolymers with specific properties were successfully prepared. This research is important for reducing petrochemical dependency.
Article
Chemistry, Multidisciplinary
Haobing Wang, Yang Yang, Masayoshi Nishiura, You-lee Hong, Yusuke Nishiyama, Yuji Higaki, Zhaomin Hou
Summary: The synthesis of self-healing polymers from simple commodity dienes, such as isoprene, using catalyst-controlled polymerization has shown to produce excellent self-healing elastomers. The self-healability is attributed to nanoscale heterogeneities formed by microphase separation of hard 3,4-segments from a flexible cis-1,4-segment matrix.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Qingde Zhuo, Xiaoxi Zhou, Takanori Shima, Zhaomin Hou
Summary: This review focuses on N-2 activation and addition to unsaturated substrates mediated by transition metal complexes, which resulted in various N-C bond formation products. The emphasis is on the reaction modes and mechanisms. It is hoped that this work will inspire further explorations in this challenging field.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Organic
Xuefeng Cong, Lin Huang, Zhaomin Hou
Summary: This Perspective focuses on recent advances in C-H functionalization with alkenes, allenes, and alkynes by half-sandwich rare-earth catalysts, including asymmetric transformations. The reaction generally proceeds through formal C-H addition to unsaturated C-C bonds, thus constituting a 100% atom-efficient route for the construction of new C-C bonds. Future outlooks in related areas are also described.
Article
Chemistry, Multidisciplinary
Aniket Mishra, Xuefeng Cong, Masayoshi Nishiura, Zhaomin Hou
Summary: Multisubstituted chiral 1-aminoindanes are important components in pharmaceuticals and bioactive molecules. The synthesis of chiral 1-aminoindanes is of great interest and importance, and the asymmetric[3 + 2] annulation of aldimines with alkenes through C-H activation is a promising method. This study reports the enantioselective [3 + 2] annulation of aromatic aldimines and alkenes via ortho-C(sp(2))-H activation using chiral half-sandwich scandium catalysts, which provides a straightforward route for the synthesis of multisubstituted chiral 1-aminoindanes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Yat-Ming So, Ching Tat To, Murali Mohan Guru, Takanori Shima, Zhaomin Hou
Summary: Carbon-carbon bond formation via coupling of two organic components is an important chemical transformation. In this study, a hydrodeoxygenative coupling of aromatic aldehydes was achieved to form bibenzyls by a titanium imide/hydride complex. The complex also demonstrated the ability to activate and functionalize N-2, as well as providing a platform for C-C bond formation using carbonyl compounds.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Organic
Masanori Takimoto, Zhaomin Hou
Summary: An efficient protocol for the carbozincation of allenamides has been developed using dialkylzinc reagents catalyzed by an NHC Cu complex. This method allows for regio- and stereoselective introduction of alkyl and zinc groups to the allenamides, leading to the formation of alkenylzinc species. These species can further undergo C-C bond-forming reactions, resulting in the synthesis of multi-substituted enamides.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Wei Zhou, Xuefeng Cong, Masayoshi Nishiura, Zhaomin Hou
Summary: The ortho-selective benzylic C(sp(3))-H alkenylation of 2-methyl tertiary anilines with internal alkynes has been achieved for the first time by using a half-sandwich scandium catalyst. This protocol provides a straightforward route for the synthesis of a new family of 2-allylaniline derivatives, featuring broad substrate scope, 100% atom-efficiency, high yields, and high chemo-, regio-, and stereoselectivity.
CHEMICAL COMMUNICATIONS
(2022)
Article
Polymer Science
Tingting Fu, Lei Jiang, Hanyang Sun, Zhaomin Hou, Fang Guo
Summary: The coordination copolymerization of polar diphenylphosphinostyrenes and isoprene using a scandium catalyst resulted in the formation of phosphine-functionalized alternating and block isoprene-styrene copolymers with different structures and polymerization modes.
