Article
Materials Science, Multidisciplinary
E. Lavrov, V. V. Melnikov, N. Abrosimov
Summary: The study revealed that the ortho-para conversion of interstitial H-2 in silicon is practically independent of the isotope composition, and interactions with nearby Si-29 nuclear spin have minimal effects on the conversion rate of molecular hydrogen in silicon.
Article
Geochemistry & Geophysics
Baojing Zhang, Tingan Zhang, Chao Zheng
Summary: This study proposes a process for smelting copper-iron alloy with copper slag and determines the suitable reduction conditions. Experimental results show that the reduction rate and metal content of copper slag can reach a high level under certain conditions. The study also finds that the reduction process is influenced by both internal diffusion and chemical reaction.
Article
Chemistry, Multidisciplinary
Xiangyun Xiao, Seok-Ho Lee, Geun-Ho Han, Kyong Ryol Tag, Jae Pyoung Ahn, Hong-Kyu Kim, Kwan-young Lee, Taekyung Yu
Summary: Structure engineering is an integrated strategy to enhance the performance of nanoparticles. In this study, clear core-shell structured Pd@Fe nanocubes with different shell thicknesses were synthesized, which showed higher H-2 conversion efficiency in direct hydrogen peroxide generation compared to ordinary Pd cubes. The advantages of the core-shell structure were attributed to the conformal growth of the Fe oxide shell and the removal of the capping agent on the Pd-Fe3O4 interface, leading to improved H-2 penetration and increased number of active sites on the inner core surface.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2023)
Article
Chemistry, Physical
Aikaterini Gemenetzi, Yiannis Deligiannakis, Maria Louloudi
Summary: This study demonstrates that photoexcited core-shell Ag-0@SiO2 nanoparticles can significantly enhance formic acid dehydrogenation, and the enhancement effect is maximized at a specific wavelength. The injection rate of hot electrons and the subsequent FADH rate can be controlled by varying the SiO2 shell thickness of Ag-0@SiO2 nanoparticles.
Article
Chemistry, Physical
Rongxue Shang, Zixuan Zhuang, Yue Yang, Gang Li
Summary: This study systematically investigates the laminar flame speeds of H-2/CH4/air mixtures with CO2 and N-2 dilution through experimental and numerical methods. The results show that the combustion transition from methane dominated to hydrogen inhibited occurs with increasing H-2 fractions, and CO2 has a stronger dilution effect on flame speeds compared to N-2. The experimental data is well-predicted by a semiempirical correlation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Materials Science, Multidisciplinary
Nazhen Liu, Fraser King, James J. Noel, David W. Shoesmith
Summary: The influence of gamma-radiation in the presence of dissolved hydrogen on the corrosion of uranium dioxide was studied, showing a suppressive effect. The reduction of U-V states due to hydrogen atoms led to the suppression of corrosion. Additionally, the production of reactive H radicals can also help inhibit the corrosion of UO2-based materials under electrochemical conditions.
Article
Chemistry, Inorganic & Nuclear
Alice Johnson, Cameron G. Royle, Claire N. Brodie, Antonio J. Martinez-Martinez, Simon B. Duckett, Andrew S. Weller
Summary: Rhodium-alkene complexes with different alkenes have been studied for their reactivity towards H-2, with only COD showing significant reaction to form a COE complex. The differences in reactivity are attributed to intramolecular alkene-assisted reductive elimination in the COD complex. Further experiments on ethene complex suggest that reductive elimination from a reversibly formed alkyl hydride intermediate is likely rate-limiting and with a high barrier.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Chunxiao Zhang, Yingjie Li, Zirui He, Jianli Zhao, Dong Wang
Summary: A hollow microtubular Fe/Mn-promoted CaO-Ca12Al14O33 bi-functional material was prepared and exhibited excellent CO2 capture and H-2 production performance in sorption enhanced water gas shift (SEWGS). The stable hollow microtubular structure improved the available adsorption and catalytic sites, while the addition of Mn enhanced CO2 affinity and Fe-Mn interaction increased redox ability. The formed compounds promoted the catalytic activity and CO2 capture capacity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Qian Li, Shuang Yang, Xingyu Lu, Tieqiang Wang, Xuemin Zhang, Yu Fu, Wei Qi
Summary: This study presents a method for designing ultrafast H-2 sensors using PdO decorated PdAu ternary hollow shells. The material exhibits high gas accessibility and surface area, and the decoration of Au and PdO reduces the energy barrier for hydrogen diffusion, resulting in an ultrafast response time of approximately 0.9 seconds.
Article
Optics
Liam H. Scarlett, Una S. Rehill, Mark C. Zammit, Nicolas A. Mori, Igor Bray, Dmitry V. Fursa
Summary: In this study, the adiabatic-nuclei molecular convergent close-coupling (MCCC) method is applied to investigate the elastic scattering and rotational excitation of H2 by 0.01-20-eV electrons. Integral cross sections are provided for all rotational transitions with |AN| 2 and Ni = 0-31 within the v = 0 vibrational level, along with differential cross sections for selected transitions. The MCCC data shows excellent agreement with available measurements and previous calculations, with the degree of agreement depending on the specific transition and incident energy. Possible reasons for the differences are suggested, and the accuracy of the MCCC data is discussed.
Article
Chemistry, Multidisciplinary
Benteng Song, Yuhong Li, Xin-Ping Wu, Fang Wang, Ming Lin, Yunhua Sun, Ai-ping Jia, Xiang Ning, Li Jin, Xiaokang Ke, Zhiwu Yu, Gang Yang, Wenhua Hou, Weiping Ding, Xue-Qing Gong, Luming Peng
Summary: ZnO plays a crucial role in many catalytic processes involving H2. By employing 17O solid-state NMR spectroscopy combined with DFT calculations, the surface structure of ZnO nanorods is unraveled and the H2 activation process is explored.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Applied
Jin Deng, Lingshuai Meng, Duo Ma, Yujie Zhou, Xianyang Wang, Xiaodong Luo, Shenfu Yuan
Summary: The development of a selective catalyst for converting biomass and plastics into H2 through steam reforming is crucial for addressing the energy crisis and global warming. In this study, Ni-Fe-Ca/H-Al bifunctional catalysts were prepared by loading Ni and Fe onto pretreated CaO/Al2O3 carriers and showed high catalytic activity for biomass and plastic steam reforming. The catalysts exhibited high H2 selectivity and low CO2 yield, and the interaction between the catalyst and carrier played a crucial role in promoting efficient steam conversion and by-product conversion to H2. The catalysts also demonstrated excellent regenerability and structural integrity after regeneration, providing a new approach for efficient H2 production from biomass and plastic steam reforming.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Nisha K. Agrawal, Soumya R. Dash, Kumar Vanka, Balaji R. Jagirdar
Summary: The abstraction of chloride from a six-coordinate complex leads to the generation of a dinitrogen complex. Addition of hydrogen to the dinitrogen complex results in the reversible coordination of H2. This H2 complex shows excellent catalytic activity for the hydrogenation of ethylene.
Article
Chemistry, Physical
Qian Xu, Marija Knezevic, Abdelghani Laachachi, Sylvain Franger, Christophe Colbeau-Justin, Mohamed Nawfal Ghazzal
Summary: The efficiency of charge transfer at the interface of transition metals loaded on TiO2 and the active reduction site play a key role in the kinetics of H2 production. In this study, the interfacial charge process of various transition metals embedded in mesoporous core-shell nanostructures was investigated. Au was found to be the most active cocatalyst, promoting both charge separation and H2 evolution. Cu(I) also exhibited similar activity and electron scavenging behavior. Ni(II) and Fe(III) were involved in charge-carrier separation but had limited contribution to H2 evolution. Only Cu(I) could compete with noble metals and exhibit electron-scavenging behavior.
Article
Chemistry, Inorganic & Nuclear
Fei Cong, Juanjuan Cheng, Han-Gook Cho, Tengfei Huang, Xuefeng Wang, Lester Andrews
Summary: The reactions of laser-ablated Ce, Sm, Eu, and Lu atoms with acetonitrile were studied by matrix infrared spectra in a neon matrix. The major product is the insertion complex (CN-M-CH3), while end-on and side-on complexes are also identified. Ce shows a significant 4f orbital contribution in bonding, while Sm and Eu show lower contributions and Lu does not involve its 4f orbital in bonding.
INORGANIC CHEMISTRY
(2021)
Correction
Instruments & Instrumentation
Seiki Baba, Hiroaki Matsuura, Takashi Kawamura, Naoki Sakai, Yuki Nakamura, Yoshiaki Kawano, Nobuhiro Mizuno, Takashi Kumasaka, Masaki Yamamoto, Kunio Hirata
JOURNAL OF SYNCHROTRON RADIATION
(2022)
Article
Chemistry, Inorganic & Nuclear
Vladimir Pelmenschikov, Chien-Hong Chen, I-Jui Hsu, Ulf-Peter Apfel, Giorgio Caserta, Lars Lauterbach, Tsai-Te Lu, Yu-Ting Tseng, Linda Iffland-Mu''hlhaus, Donato Calabrese, Yu-Che Chang, Konstantin Laun, Chih-Wen Pao, Ilya Sergueev, Yoshitaka Yoda, Wen-Feng Liaw
Summary: Efforts are being made to develop earth-abundant metal catalysts for dehydrogenation/hydrolysis of amine boranes. In this study, complex 3-K-crown was explored as a pre-catalyst for the dehydrogenation of DMAB, and the transformation of 3-K-crown into intermediate A during H-2 generation was supported by experimental and computational results. The substrate-gated transformation of pre-catalyst 3 into intermediate A was also observed in the reaction of complex 4-Na-crown with CO as an alternative synthetic route.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Vladimir Pelmenschikov, Delfim Ferreira, Sofia S. Venceslau, Peter Hildebrandt, Ines A. . C. Pereira, Smilja Todorovic, Smilja Todorovic
Summary: In this study, resonance Raman spectroscopy and density functional theory calculations were used to investigate the structural, electronic, and vibrational properties of the noncubane [4Fe-4S] cluster in heterodisulfide reductase (HdrB). Homology modeling was employed to predict the protein environment of the neighboring clusters in DvHdrB. The results showed that the oxidized [4Fe-4S](3+) cluster adopts a closed conformation in the absence of substrate, but transitions to an open structure upon substrate coordination, accompanied by a ligand switch. This study provides valuable insights for future research on enzymes with this unconventional cofactor.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Konrad Kretschmar, Vladimir Pelmenschikov, Martin Kaupp, Thomas Braun, Philipp Wittwer, Simon Rachor, Jesvita Cardozo
Summary: A set of bimetallic complexes based on iridium and rhodium with various bridging ligands were synthesized and studied for catalytic hydrodefluorination reactions using molecular hydrogen and sodium tert-butoxide. The effects of ligand variation, nuclearity, and metal identity were investigated to optimize the hydrodefluorination process.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Bo-Hau Chen, Jun-Jia Xu, Wei-Ren Lai, Chung-Kai Chang, Jeng-Lung Chen, Jyh-Fu Lee, Jin-Ming Chen, Hwo-Shuenn Sheu, Jey-Jau Lee, Yoshiki Kubota, Ming-Hsi Chiang, Yasutaka Kitagawa, Yu-Chun Chuang, I-Jui Hsu
Summary: Two cobalt(II) halide complexes, [Co(Htrz)Cl-2](n) and {[Co(Htrz)(2)(trz)]BF4}(n), with 1,2,4-triazole as a ligand, were synthesized. The structures of these complexes were determined using extended x-ray absorption fine structure (EXAFS) and powder x-ray diffraction (XRD). Both complexes form one-dimensional polymeric chains with Co center dot center dot center dot Co distances of 3.3521(2) A and 3.8629(2) A, respectively. The analysis of Co L-II,L-III-edge XAS indicates that the Co(II) in these complexes are in a high spin state with t(2g)(5)e(g)(2) configuration. The broken-symmetry DFT calculations reveal that the antiferromagnetic coupling state of Co center dot center dot center dot Co is the most stable state in both complexes, with coupling constants of -0.32 cm(-1) and -3.70 cm(-1) for complexes 1 and 2, respectively. The antiferromagnetic interaction is achieved through triazole ligands based on the distances of Co center dot center dot center dot Co and coupling constants.
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Ting Yi Lai, Chang-Ting Chen, Kai-Ti Chu, Su-Ying Chien, Tiow-Gan Ong, Ming-Hsi Chiang
Summary: A new 3Fe4S cluster related to M-cluster of Mo-nitrogenase is reported. It is synthesized from the structural rearrangement of [K(THF)(2)][(mu,kappa(2)-bdt)Fe-2(mu-PPh2)(CO)(5)] under visible light irradiation. The Fe-hydride species (1H) with bridging hydride group is generated and characterized by H-1-NMR spectroscopy and DFT calculation. Complex 1 exhibits reversible reduction and oxidation processes in CH3CN solution.
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Isabel Bogacz, Hiroki Makita, Philipp S. S. Simon, Miao Zhang, Margaret D. D. Doyle, Ruchira Chatterjee, Thomas Fransson, Clemens Weninger, Franklin Fuller, Leland Gee, Takahiro Sato, Matthew Seaberg, Roberto Alonso-Mori, Uwe Bergmann, Vittal K. K. Yachandra, Jan Kern, Junko Yano
Summary: X-ray crystallography and X-ray spectroscopy are important in understanding the interplay of structural changes in proteins and chemical changes at metal active sites. In this study, we developed methods for X-ray absorption spectroscopy (XAS) to study dilute biological samples using X-ray free electron lasers. Our focus was on Photosystem II (PS II), a membrane protein complex, which catalyzes water oxidation using a Mn4CaO5 cluster. We describe our method for collecting XAS data using PS II samples with a low Mn concentration, employing a drop-on-demand sample delivery method.
PURE AND APPLIED CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jared C. Paris, Sha Hu, Aiwen Wen, Andrew C. Weitz, Ronghai Cheng, Leland B. Gee, Yijie Tang, Hyomin Kim, Arturo Vegas, Wei-chen Chang, Sean J. Elliott, Pinghua Liu, Yisong Guo
Summary: This study reports the first observation of a spin iron(IV) species in non-heme iron enzymes, which enables the formation of C-S bond catalyzed by OvoA in Methyloversatilis thermotolerans. This finding paves the way for understanding the mechanism of enzymatic oxidative C-S bond formation in the OSHA biosynthesis pathway.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Augustin Braun, Leland B. Gee, Michael W. Mara, Ethan A. Hill, Thomas Kroll, Dennis Nordlund, Dimosthenis Sokaras, Pieter Glatzel, Britt Hedman, Keith O. Hodgson, A. S. Borovik, Michael L. Baker, Edward I. Solomon
Summary: Fe K-edge XAS is widely used for studying high-valent iron intermediates in catalysts. The 4p-mixing into the 3d orbitals complicates the analysis, but understanding it correctly enables deeper insights into the structure and reactivity. This study reveals that the loss of inversion in the equatorial plane leads to 4p mixing into the 3dx2-y2,xy orbitals, providing structural insights for distinguishing 6- vs 5-coordinate active sites. Furthermore, the study investigates the electronic structure of Fe(IV)=O active sites and their reactivity selectivity through O K-edge XAS.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Leland B. Gee, Jinkyu Lim, Thomas Kroll, Dimosthenis Sokaras, Roberto Alonso-Mori, Chien-Ming Lee
Summary: We utilized hard X-ray spectroscopic methods to identify the structural features and reaction mechanisms of two photolabile {FeNO}(6) complexes, providing a foundation for future research.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Hao-Wen Kang, Yu-Chiao Liu, Wei-Kai Shao, Yu-Chen Wei, Chi-Tien Hsieh, Bo-Han Chen, Chih-Hsuan Lu, Shang-Da Yang, Mu-Jeng Cheng, Pi-Tai Chou, Ming-Hsi Chiang, Yao-Ting Wu
Summary: The synthesis, structures, and properties of highly twisted alkenes were investigated. The rotation of the central C = C bonds in these compounds is as facile as the rotation of aryl-aryl bonds in 2-fluorobiphenyl. The compounds exhibit broad photoabsorption range, reduced HOMO-LUMO gap, and small singlet-triplet energy gap.
NATURE COMMUNICATIONS
(2023)
Article
Biochemical Research Methods
Hiroaki Matsuura, Naoki Sakai, Sachiko Toma-Fukai, Norifumi Muraki, Koki Hayama, Hironari Kamikubo, Shigetoshi Aono, Yoshiaki Kawano, Masaki Yamamoto, Kunio Hirata
Summary: In macromolecular structure determination using X-ray diffraction from multiple crystals, hierarchical clustering analysis (HCA) has been effective in classifying polymorphous data sets with a certain threshold, allowing for the identification of polymorphs in data sets with unknown structural heterogeneity. Additionally, polymorphs can also be detected in single crystals using the continuous helical scheme.
ACTA CRYSTALLOGRAPHICA SECTION D-STRUCTURAL BIOLOGY
(2023)
Article
Chemistry, Physical
Rohan Paste, Shenghan Li, Jui-Han Fu, Yu-Hsiang Chiang, Arif I. Inamdar, Ming-Hsi Chiang, Vincent Tung, Hong-Cheu Lin, Chih Wei Chu
Summary: Stable lithium-sulfur batteries have the potential to be the next generation of stable energy-storage devices. This study introduces a modified separator (MC separator) with crumpled MoS2 nanosheets, which can adsorb lithium polysulfides and provide additional reaction sites, leading to enhanced specific capacity and cycling stability of the battery.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Inorganic & Nuclear
Chang-Chih Hsieh, Po-Kuang Liao, Chia-Wei Chen, Ming-Hsi Chiang, Yih-Chern Horng
Summary: In this study, six new pyrazolylamidino Cu(II) complexes were synthesized from the direct reaction of Cu(X)(2) salts and pyrazole in nitrile solution. The complexes were characterized using various spectroscopic techniques and X-ray crystallographic analysis. The crystal structures of the complexes revealed diverse supramolecular assemblies through different interactions. EPR results indicated weak magnetic couplings between Cu(II) centers. The study also proposed a plausible synthetic path for synthesizing pyrazolylamidino Cu(II) complexes.
DALTON TRANSACTIONS
(2023)
Meeting Abstract
Biochemistry & Molecular Biology
Courtney Petersen, Leland Gee, Adam Jenkins, Hongxin Wang, Simon George, Yoshitaka Yoda, Nobutomo Nagasawa, Hiroaki Matsuura, Hannah Shafaat, Stephen Cramer, Matthew Thompson
