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A special column highlighting young scientists at institute of chemistry, Chinese Academy of Sciences (ICCAS)

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Chinese Chemical Letters 2018年第3期29卷 343-344页

作者： Zhixun,Luo Zhenzhong Yang chinese academy of sciences state key laboratory for structural chemistry of unstable and stable species institute of chemistrychinese academy of sciences Beijing 100190 China

Just seeing off the BOth anniversary of the institute of chemistry, Chinese Academy of Sciences （ICCAS）, we are here with pleasure to conduct A Special Column for Young Scientists at ICCAS published in Chinese chemistry Letters （CCL） endeavoring to disseminate positive energy of several enthusiastic chemists and spread their recent research to the global scientific community.

关键词： ICCAS A special column highlighting young scientists at institute of chemistry Chinese Academy of Sciences

Multicomponent transition metal oxides and(oxy)hydroxides for oxygen evolution

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Nano Research 2023年第2期16卷 1913-1966页

作者： Jingyi Han Jingqi Guan institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China

Oxygen evolution reaction(OER)is the core electrode reaction in energy-related technologies,such as electrolytic water,electrocatalytic carbon dioxide reduction,rechargeable metal-air batteries,and renewable fuel cells.Development of well-stocked,cost-effective,and high-performance OER electrocatalysts is the key to the improvement of energy efficiency and the large-scale commercial implementation of these technologies.Multicomponent transition metal oxides and(oxy)hydroxides are the most promising OER catalysts due to their low cost,adjustable structure,high electrocatalytic activity,and outstanding durability.In this review,a brief overview about the mechanisms of OER is first offered,accompanied with the theory and calculation criteria.Then,the latest advances in the rational design of the related OER electrocatalysts and the modulation of the electronic structure of active sites are comprehensively summarized.Specifically,various strategies(including element doping,defect engineering,and fabrication of binderless catalysts)used to improve the OER performance are detailedly discussed,emphasizing the structure–function relationships.Finally,the challenges and perspectives on this promising field are proposed.

关键词： oxyhydroxide mixed oxide oxygen evolution reaction single-atom catalyst water splitting

Design and Synthesis of Spirochroman-2-on-4,1'-indan-7'-ol and Its Application for Synthesizing Chiral Monophosphinite Ligands

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Chinese Journal of chemistry 2023年第22期41卷 2988-2994页

作者： Yang-Ming Zhang Shu-Min Guo Qing-Xian Wang Xiao-Jie Zheng Jian-Hua Xie Qi-Lin Zhou StateKeyLaboratoryand institute of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

The design and synthesis of spirochroman-2-on-4,1'-indan-7'-ol(SCIOL)and its application for synthesizing chiral monophosphinite ligands are reported.The synthesis features a tandem double Friedel-Crafts reaction/lactonization to construct the spiro framework and the desired racemic SCiOL was obtained via 6 steps with a total yield of 44.5%.Using an inclusion resolution with N-benzylcinchonidinium chloride,the optical SCiOL could be obtained in good yields on a gram scale.The preliminary studies indicated that the corresponding chiral spiro monophosphinite ligands exhibit high catalytic activity and enantioselectivity(up to 94%ee)in the rhodium-catalyzed asymmetric hydrogenation of N-acetyl dehydroamino esters.These outcomes highlight the significant potential of SCiOLas a useful framework forthedevelopment of chiral spiro ligands.

关键词： Asymmetric catalysis Ligand design Hydrogenation Monophosphinites Spiro ligands

Preliminary studies on the stability of arsenolipids:Implications for sample handling and analysis

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Journal of Environmental Sciences 2016年第11期28卷 97-103页

作者： Muslim Khan Kevin A.Francesconi institute of chemistry-Analytical chemistry University of Graz

Human health risk assessments concerning arsenic are now estimating exposure through food in addition to exposure through drinking water. Intrinsic to this assessment is sample handling and preparation that maintains the arsenic species in the form that they occur in foods. We investigated the stability of three arsenolipids（two arsenic fatty acids, As FA-362 and As FA-388, and one arsenic hydrocarbon As HC-332）, common constituents of fish and algae, relevant to sample storage and transport, and to their preparation for quantitative measurements. The fate of the arsenolipids was followed by high performance liquid chromatography/electrospray triple quadruple mass spectrometry（HPLC/ESIMS） analyses.Storage of the compounds dry as pure compounds or mixed in fish oil at up to 60？C did not result in significant changes to the compounds, although losses were observed by apparent adsorption onto the plastic walls of the polypropylene tubes. No losses occurred when the experiment was repeated with glass tubes. When the compounds were stored in ethanol for up to 15 days under acidic, neutral, or alkaline conditions（each at room temperature）, no significant decomposition was observed, although esterification of the fatty acids occurred at low p H. The compounds were also stable during a sample preparation step involving passage through a small silica column. The results indicate that these typical arsenolipids are stable when stored in glass at temperatures up to 60？C for at least 2 days, and that,consequently, samples of food or extracts thereof can be transported dry at ambient temperatures, i.e. without the need for cool conditions.

关键词： Arsenolipids Stability Mass spectrometry

Carbon-supported CoS_(4)-C single-atom nanozyme for dramatic improvement in CO_(2)electroreduction to HCOOH:A DFT study combined with hybrid solvation model

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中国化学快报:英文版 2023年第8期34卷 449-453页

作者： Hao Sun Jingyao Liu institute of Theoretical chemistry College of ChemistryJilin UniversityChangchun 130023China

Single-atom nanozymes(SANs)have attracted extensive attention due to their characteristics of both single-atom catalysts(SACs)and enzymes.Using spin-polarized density functional theory(DFT)calculations combined with the hybrid solvation model,this work designed a series of carbon-supported Group VIII transition metals TMS_(4)-C SANs,similar to the TMS_(4)active center of formate dehydrogenase(FADH),aiming to develop highly efficient SANs for CO_(2)electroreduction.DFT calculations show that compared with TMN4-C,TMS_(4)-C have FADH-like feature,which can selectively reduce CO_(2)to formic acid.Particularly,CoS4-C is the most promising SAN for CO_(2)reduction,with a low limiting potential of-0.07 V,which exceeds most reported catalysts.Two descriptors of TMX4-C(X=N,S)based on intrinsic and electronic structure properties were proposed to shed light on the origin activity of candidates.The findings presented here will provide new insights into the design of novel enzyme-like catalysts for electrochemical CO_(2)reduction.

关键词： Single-atom catalysts Nanozymes Electrocatalysis CO_(2)reduction Density functional theory

Wood pulp industry by-product valorization for acrylate synthesis and bio-based polymer development via Michael addition reaction

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生物质资源与工程(英文) 2023年第3期8卷 265-279页

作者： Ralfs Pomilovskis Eliza Kaulina Inese Mierina Arnis Abolins Olga Kockova Anda Fridrihsone Mikelis Kirpluks Polymer Laboratory Latvian State Institute of Wood ChemistryRiga LV-1006Latvia institute of Technology of Organic chemistry Faculty of Materials Science and Applied ChemistryRiga Technical UniversityRiga LV-1048Latvia institute of Macromolecular chemistry CAS Prague 16200Czech Republic

It is crucial to adapt the processing of forest bio-resources into biochemicals and bio-based ad-vanced materials in order to transform the current economic climate into a greener economy.Tall oil,as a by-product of the Kraft process of wood pulp manufacture,is a promising resource for the extraction of various value-added products.Tall oil fatty acids-based multifunctional Michael acceptor acrylates were developed.The suitability of developed acrylates for polymerization with tall oil fatty acids-based Michael donor acetoacetates to form a highly cross-linked polymer ma-terial via the Michael addition was investigated.With this novel strategy,valuable chemicals and innovative polymer materials can be produced from tall oil in an entirely new way,making a significant contribution to the development of a forest-based bioeconomy.Two different tall oil-based acrylates were successfully synthesized and characterized.Synthesized acrylates were successfully used in the synthesis of bio-based thermoset polymers.Obtained polymers had a wide variety of mechanical and thermal properties(glass transition temperature from-12.1 to 29.6°C by dynamic mechanical analysis,Young’s modulus from 15 to 1760 MPa,and stress at break from 0.9 to 16.1 MPa).Gel permeation chromatography,Fourier-transform infrared(FT-IR)spectroscopy,matrix-assisted laser desorption/ionization-time of flight mass spectrometry,and nuclear magnetic resonance were used to analyse the chemical structure of synthesized acrylates.In addition,various titration methods and rheology tests were applied to characterize acrylates.The chemical composition and thermal and mechanical properties of the developed polymers were studied by using FT-IR,solid-state nuclear magnetic resonance,thermal gravimetric analy-sis,differential scanning calorimetry,dynamic mechanical analysis,and universal strength testing apparatus.

关键词： Tall oil fatty acid Fatty acids-based michael acceptor Bio-based acrylate Michael addition Bio-based polymer

Emerging analytical methods to characterize zeolite-based materials

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National Science Review 2022年第9期9卷 47-66页

作者： Sophie H.van Vreeswijk Bert M.Weckhuysen Inorganic chemistry and Catalysis Debye Institute for NanomaterialsUtrecht University

Zeolites and zeolitic materials are,through their use in numerous conventional and sustainable applications,very important to our daily lives,including to foster the necessary transition to a more circular society.The characterization of zeolite-based materials has a tremendous history and a great number of applications and properties of these materials have been discovered in the past decades.This review focuses on recently developed novel as well as more conventional techniques applied with the aim of better understanding zeolite-based materials.Recently explored analytical methods,e.***.atom probe tomography,scanning transmission X-ray microscopy,confocal fluorescence microscopy and photo-induced force microscopy,are discussed on their important contributions to the better understanding of zeolites as they mainly focus on the micro-to nanoscale chemical imaging and the revelation of structure-composition-performance relationships.Some other techniques have a long and established history,e.***.nuclear magnetic resonance,infrared,neutron scattering,electron microscopy and X-ray diffraction techniques,and have gone through increasing developments allowing the techniques to discover new and important features in zeolite-based materials.Additional to the increasing application of these methods,multiple techniques are nowadays used to study zeolites under working conditions(i.***.the in situ/operando mode of analysis) providing new insights in reaction and deactivation mechanisms.

关键词： catalysis zeolites spectroscopy microscopy structure–composition–performance relationships

Reversible Insertion of CO_(2)into a Bis(formazanate)Magnesium Complex

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CCS chemistry 2023年第6期5卷 1277-1284页

作者： Da Jin Xiaofei Sun Alexander Hinz Peter W.Roesky institute for Inorganic chemistry Karlsruhe Institute of Technology76131 Karlsruhe

The capture,storage,and release of CO_(2)is one of the most pressing issues in chemistry.Herein,we designed bis(formazanate)magnesium complexes as precursors,which were synthesized by straightforward transamination between the neutral formazan[PhNNC(4-tBuPh)NNHPh](LH)and[Mg{N(SiMe_(3))_(2)}_(2)].Depending on the solvent,either the homoleptic complex[L_(2)Mg]or the thf-coordinated complex[L_(2)Mg(thf)]was isolated.Reaction of the solvent-free complex[L_(2)Mg]with CO_(2)led to stoichiometric insertion into one of the four Mg–Nbonds with concomitant rearrangement of the ligand scaffold which adopts a trinuclear cagelike structure.The insertion reaction is reversible depending on thermolysis or treatment with tetrahydrofuran,which is corroborated by density functional theory calculations.This showcases the first example of reversible uptake of CO_(2)by an s-block coordination compound.

关键词： reversibility CO_(2)activation formazanate magnesium s-block chemistry

Dual-radical-based molecular anisotropy and synergy effect of semi-conductivity and valence tautomerization in a photoswitchable coordination polymer

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National Science Review 2023年第6期10卷 200-214页

作者： Jing-Wei Dai Yu-Qin Li Zhao-Yang Li Hai-Tao Zhang Carmen Herrmann Shohei Kumagai Marko Damjanovi? Markus Enders Hiroyuki Nojiri Masakazu Morimoto Norihisa Hoshino Tomoyuki Akutagawa Masahiro Yamashita State Key Laboratory of Medicinal Chemical Biology Nankai University School of Materials Science and Engineering Nankai University institute of Inorganic and Applied chemistry University of Hamburg Department of chemistry Graduate School of Science Tohoku University institute of Inorganic chemistry University of Heidelberg institute for Materials Research Tohoku University Department of chemistry Rikkyo University institute of Multidisciplinary Research for Advanced Materials (IMRAM) Tohoku University

Organic radicals are widely used as linkers or ligands to synthesize molecular magnetic materials.However,studies regarding the molecular anisotropies of radical-based magnetic materials and their multifunctionalities are rare.Herein,a photoisomerizable diarylethene ligand was used to form{[CoⅢ(3,5-DTSQ·-)(3,5-DTCat2-)]2(6F-DAE-py2)}·3CH3CN·H2O(o-1·3CH3CN·H2O,6F-DAE-py2=1,2-bis(2-methyl-5-(4-pyridyl)-3-thienyl)perfluorocyclopentene),a valence-tautomeric(VT) coordination polymer.We directly observed dual radicals for a single crystal using high-field/-frequency(～13.3 T and～360 GHz) electron paramagnetic resonance(EPR) spectroscopy along the c-axis,which was further confirmed by angle-dependent Q-band EPR spectroscopy.Moreover,a conductive anomaly close to the VT transition temperature was observed only when probes were attached at the ab plane of the single crystal,indicative of synergy between valence tautomerism and conductivity.Structural anisotropy studies and density functional theory(DFT) calculations revealed that this synergy is due to electron transfer associated with valence tautomerism.This study presents the first example of dual-radical-based molecular anisotropy and charge-transfer-induced conductive anisotropy in a photoswitchable coordination polymer.

关键词： valence tautomerization charge transfer photo switching diradical coordination polymer