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Differentially-grown cobalt regulators cooperatively involved in the tandem catalysis for high-yield production of second amines

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Nano Research 2024年第4期17卷 2444-2450页

作者： Jinhui Xu Xiao Wang Ying Wang Fei Wang Lingling Zhang Wenjie Cui Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Department of chemistry Tsinghua UniversityBeijing 100084China

One-pot tandem catalysis has been regarded as one of the most atomic economic ways to produce secondary amines,the important platform molecules for chemical synthesis and pharmaceutical manufacture,but it is facing serious issues in overall *** promotional effects are highly desired for boosting the activity and regulating the selectivity of conventional tandem *** this work,we report a high-performance tandem catalyst with maximized synergistic effect among each counterpart by preciously manipulating the spatial structure,which involves the active CeO_(2)/Pt component as kernel,the densely-coated N-doped C(NC)layer as selectivity controller,and the differentially-grown Co species as catalytic performance *** comprehensive investigations,the unique growth mechanism and the promotion effect of Co regulators are ***,the surface-landed Co clusters(Cocs)are crucial to selectivity by altering the adsorption configuration of benzylideneaniline ***,the inner Co particles(Cops)are essential for activity by denoting their electrons to neighboring *** from the unique promotion effect,a remarkably-improved catalytic efficiency(100%nitrobenzene conversion with 94%N-benzylaniline selectivity)is achieved at a relatively low temperature of 80℃,which is much better than that of CeO_(2)/Pt(100%nitrobenzene conversion with 12%N-benzylaniline selectivity)and CeO_(2)/Pt/NC(35%nitrobenzene conversion with 94%benzylideneaniline selectivity).

关键词： tandem catalysis CeO_(2) hierarchical structure heterogeneous catalyst dual-site materials

Antimony oxides-protected ultrathin Ir-Sb nanowires as bifunctional hydrogen electrocatalysts

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Nano Research 2024年第3期17卷 1042-1049页

作者： Bingyan Xu Xuan Huang Shangheng Liu Zhiwei Hu Cheng-Wei Kao Ting-Shan Chan Hongbo Geng Ying Zhang Xiaoqing Huang Country State Key Laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Max Planck institute for Chemical Physics of Solids Dresden 01187Germany “National Synchrotron Radiation Research Center” Hsinchu 30076TaiwanChina School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Developing electrocatalysts with fast kinetics and long-term stability for alkaline hydrogen oxidation reaction(HOR)and hydrogen evolution reaction(HER)is of considerable importance for the industrial production of green and sustainable ***,an ultrathin Ir-Sb nanowires(Ir-Sb NWs)protected by antimony oxides(SbO_(x))was synthesized as an efficient bifunctional catalyst for both HOR and HER under alkaline *** from the much higher mass activities of Ir-Sb nanowires than those of Ir nanowires(Ir NWs)and commercial Pt/C,the SbO_(x) protective layer also contributes to the maintenance of morphology and anti-CO poisoning ability,leading to the long-term cycling performance in the presence of ***,the Ir-Sb NW/SbO_(x) exhibits the highest catalytic activities,which are about 3.5 and 4.8 times to those of Ir NW/C and commercial Pt/C toward HOR,*** work provides that the ultrathin morphology and H_(2)O-occupied Sb sites can exert the intrinsic high activity of Ir and effectively optimize the absorption of OH*both in alkaline HER/HOR electrolysis.

关键词： Ir nanowire amorphous antimony oxides bifunctional mechanism hydrogen evolution reaction hydrogen oxidation reaction

Injectable chitosan hydrogels loaded with antioxidant agent as first-aid dressings for second-degree burn wounds

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Science China(Technological Sciences) 2024年第3期67卷 891-901页

作者： REN Hui ZHANG Zhen LU KaiLun SHEN YuanYuan HE ChaoLiang CHEN XueSi CAS Key Laboratoryof Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Burn wounds are destructive skin traumas typically of irregular shape and large area. Prone to infection, they require frequent dressing replacement, and painless removal of dressings from burn wounds remains a major challenge. This study focuses on the dynamic characteristics and treatment difficulty of burn wounds. Hydrogel dressings based on glycol chitosan and propionaldehyde-or benzaldehyde-terminated 4-arm poly(ethylene glycol) were designed on the basis of Schiff base cross-linking networks. The hydrogels exhibited shape-adaptability, self-healing and fast-degradation properties, which makes these hydrogels suitable for burn wounds. Salvianolic acid B(SaB)-loaded hydrogel exhibited good antioxidant properties in vitro. In a rat model of deep second-degree burn wounds, the SaB-loaded hydrogel could quickly reduce wound temperature, regulate wound oxidant microenvironment, promote angiogenesis, and accelerate wound healing. Thus, the drug-loaded hydrogel shows significant potential as a first-aid dressing for treatment of burn wounds.

关键词： hydrogel dressing fast-degradation shape-adaptability stress relaxation burn wound treatment

Heterocatalytic ethylene methoxycarbonylation via a pseudo-hydride pathway over Pt_(1)/MoS_(2)

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Science China chemistry 2024年第8期67卷 2427-2428页

作者： Bo-Hang Zhao Bin Zhang institute of Molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Ethylene (C2H4) methoxycarbonylation (EMC) with CO and methanol (CH3OH) to methyl propanoate (MP) is industrially important due to its 100% atom efficiency [1].However, the heavy reliance on homogeneous Pd-based catalysts and strong acid media over commercial EMC processes still causes economic and environmental concerns [2]. At present, supported single-atom catalysts (SACs) can serve as bridges for accessing homogeneous catalysts in traditional heterogeneous catalytic processes.

关键词： processes. catalytic hydride

High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines

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Chinese Journal of Polymer Science 2024年第2期42卷 188-201,I0007页

作者： Chantsalnyam Bariashir Qiu-Yue Zhang Bayasgalan Ulambayar Gregory A.Solan Tong-Ling Liang Wen-Hua Sun institute of chemistry and Chemical Technology Mongolian Academy of SciencesUlaanbaatar13330Mongolia Key Laboratory of Engineering Plastics and Beijing National Laboratory for Molecular Science Institute of ChemistryChinese Academy of SciencesBeijing100190China Department of chemistry University of LeicesterUniversity RoadLeicesterLE17RHUK State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China

The N,N,N'-ferrous chloride complexes,[2-{CMeN(2,4-(CHPh)_(2)-6-FC_(6)H_(2))}-6-(CMeNAr)C_(5)H_(3)N]FeCl_(2)(Ar=2,6-Me_(2)C_(6)H_(3) Fe1,2,6-Et_(2)C_(6)H_(3)Fe2,2,6-^(i)Pr_(2)C_(6)H_(3) Fe3,2,4,6-Me_(3)C_(6)H_(2) Fe4 and 2,6-Et_(2)-4-MeC_(6)H_(2) Fe5),each possessing one N-2,4-dibenzhydryl-6-fluorophenyl group,were readily synthesized from their respective unsymmetrical bis(imino)pyridines,*** identification of Fe2 highlighted the variation in the steric properties provided by the dissimilar N-aryl *** pre-treatment with either MAO or MMAO,complexes Fe1-Fe5 all displayed,at an operating temperature of 80℃,high activities for ethylene polymerization with levels falling in the order:Fe4> Fe1> Fe5> Fe2> ***,Fe4/MAO displayed the highest activity of 1.94×10^(7) g_(PE)·mol_(Fe)^(-1)·h^(-1) of the study with only a modest loss in performance at 90℃.Generally,the resulting polyethylenes were highly linear(T_(m) range:122-132℃),narrowly disperse and of low molecular weight(M_(w) range:6.73-46.04kg·mol^(-1)),with the most sterically hindered Fe3 forming the highest molecular weight polymer of the ***-group analysis by ^(1)H-and ^(13)CNMR spectroscopy revealed saturated alkyl(n-propyl and i-propyl) and unsaturated vinyl chain ends indicative of the role of both β-H elimination and chain transfer to aluminum as termination *** comparison with previou sly reported iron precatalysts with similar tridentate ligand skeletons,it is evident that the introduction of a large benzhydryl group in combination with a fluorine as the ortho-substituents of one N-aryl group has the effect of enhancing thermal stability of the iron polymerization catalyst whilst maintaining appreciable polymer molecular weight.

关键词： Iron catalyst Ethylene polymerization Linear polyethylene Fluoride effect Thermal stability

Rapid and chemoselective imidation of sulfides in aqueous buffer enabled by a novel guanidine-derived N-O reagent

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Science China chemistry 2024年第6期67卷 1929-1934页

作者： Hanzheng Li Long Xu Jiajia Dong Key Laboratory of Organofluorine chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai200032China institute of Translational Medicine National Facility for Translational Medicine(Shanghai)Shanghai Jiao Tong UniversityShanghai200240China School of chemistry and Chemical Engineering Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai200240China Shanghai Artificial Intelligence Laboratory Shanghai200232China

Herein we report the facile synthesis of a series of novel N-O reagents and identify N′-di-Boc-N′′-[(mesitylsulfonyl)oxy]-guanidine as an efficient imidating *** reagent is synthetically scalable and bench-stable,yet it shows unprecedented reactivity and chemoselectivity towards S(II)in buffer/hexafluoroisopropanol(HFIP)system,to generate a new class of Nguanyl *** transformation of N-guanyl sulfilimines to N-guanyl sulfoximines provides us a chance to investigate these rarely reached compounds,which are shown to be versatile precursors to a variety of N-heterocyclic and *** work provides an addition to the tool box of both sulfur imidation and guanidine synthesis,especially for the need of rapid and selective modifications of sulfur(II)center under biocompatible conditions.

关键词： sulfur imidation N-O reagent

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Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

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Nano-Micro Letters 2024年第3期16卷 333-350页

作者： Xudong Li Zhuomin Qiang Guokang Han Shuyun Guan Yang Zhao Shuaifeng Lou Yongming Zhu Department of Applied chemistry Harbin Institute of Technology at WeihaiWeihai 264209People’s Republic of China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen *** extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still ***,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox *** entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction *** a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts *** encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

关键词： Lithium-oxygen batteries KCoMnNiMgZnF_(3)-HEC perovskite fluoride Entropy effect Catalytic kinetics d-p orbital hybridization

Tuning microstructures of Mg-Ce-Ni hydrogen storage alloys via Cu and carbon nanotube additions

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Nano Research 2024年第8期17卷 7203-7211页

作者： Linlin Zhang Liang Xiong Bingyang Gao Qingyun Shi Ying Wang Zhiya Han Zhenhua Zhang Chunli Wang Limin Wang Yong Cheng State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Purification Equipment Research institute of CSIC Handan 056002China

Mg-based alloys are regarded as highly promising materials for hydrogen *** significant improvements of the properties for Mg-based alloys,challenges such as slow hydrogen absorption/desorption kinetics and high thermodynamic stability continue to limit their practical *** this study,to assess hydrogen storage alloys with enhanced properties,incorporating both internal microstructure modulation through the preparation of amorphous/nanocrystalline structures and surface property enhancement with the addition of Cu and carbon nanotubes(CNTs),the kinetic properties of activation and hydrogenation,thermodynamic properties,and dehydrogenation kinetics are *** results reveal a complementary interaction between the added Cu and CNTs,contributing to the superior hydrogen storage performance observed in sample 7A-2Cu-1CNTs with an amorphous/nanocrystalline structure compared to the other experimental ***,the samples are fully activated after the initial hydrogen absorption and desorption cycle,demonstrating outstanding hydrogenation kinetics under both high and low temperature experimental *** noteworthy is that the hydrogen absorption exceeds 1.8 wt.%within one hour at 333 ***,the activation energy for dehydrogenation is decreased to 64.71 kJ·mol^(–1).This research may offer novel insights for the design of new-type Mg-based hydrogen storage alloys,which possess milder conditions for hydrogen absorption and desorption.

关键词： Mg-Ni-Ce alloy hydrogen storage amorphous/nanocrystalline structure kinetics Cu and carbon nanotubes(CNTs)codoping

Selective control of secondary alcohols upgrading using Ir-catalyzed cross-coupling strategy

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Science China chemistry 2024年第3期67卷 914-921页

作者： Siqi Yang Zeye Lu Jiale Ji Qingshu Zheng Tao Tu Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China Frontiers Science Center for Transformative Molecules School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The selective coupling of alcohols is a fascinating yet challenging approach for upgrading alcohols. Herein, we accomplished the controlled production of β-disubstituted ketones or upgraded secondary alcohols via the Ir-catalyzed cross-coupling of secondary alcohols in excellent yields with broad substrate scopes. This selective control was achieved by using an in-situ generated monoNHC-Ir or a tris-NHC-Ir complex as the catalysts, respectively. Mechanistic studies revealed that the delicate balance between dehydrogenation and hydrogenation abilities of these bifunctional catalysts is crucial for achieving different selectivity. The tris-NHC-Ir complex effectively facilitated dehydrogenation of alcohols and hydrogenation of intermediates, leading to the desired upgraded secondary alcohols. Conversely, the high dehydrogenation ability of the mono-NHC-Ir complex promoted the conversion of formed secondary alcohols back to ketones.

关键词： cross-coupling hydrogen-borrowing NHC-Ir complexes selectivity control upgrading of alcohols