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Relay C（sp3）-H bond trifluoromethylthiolation and amidation by visible light photoredox catalysis

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Science China chemistry 2024年第11期67卷 3844-3850页

作者： Junheng Liu Suqi Yang Shunruo Yao Chengjian Zhu Yong Liu Weipeng Li Jin Xie state key laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green Catalysis Center College of Chemistry Zhengzhou University state key laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Nanjing Bready Advanced Materials Technology Co. Ltd. state key laboratory of natural Medicines China Pharmaceutical University

Selective functionalization of C（sp3）–H bonds is a straightforward and practical method to construct complex molecule skeletons. In this field, direct transformation of unactivated C（sp3）–H bonds into C（sp3）–SCF3architectures is still a great *** report a highly selective trifluoromethylthiolation of unactivated aliphatic C（sp3）–H bonds by combination of proton-coupled electron transfer（PCET） and hydrogen atom transfer（HAT） strategy. A wide range of structurally diverse alkyl trifluoromethyl sulfides are obtained. Furthermore, the use of two different photocatalysts can realize an unprecedented trifluoromethylthiolation and amidation cascade of different C（sp3）–H bonds. It can afford a good access to bifunctionalized molecules in synthetically useful yields.

关键词： photoredox catalysis C–H activation trifluoromethylthiolation amidation PCET

Chemoselective and Living/Controlled Polymerization of Alkenyl Methacrylates by the Phosphonium Ylide/Organoaluminum Lewis Pairs

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Chinese Journal of Polymer Science 2024年第2期42卷 159-167,I0005页

作者： Zhi-Kang Chen Wu-Chao Zhao Yi-Ling Zhao Cong-Lei Liu Liu-Yin Jiang Yue-Tao Zhang Hong-Ping Zhu state key laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China state key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun130012China

Chemoselective,living/controlled polymerizations of allyl methacrylate(AMA) and vinyl methacrylate(VMA) with/without methyl methacrylate(MMA) by using the phosphonium ylide/organoaluminum based Lewis pairs(LPs) have been *** P-ylide-2/AIMe(BHT)_(2)(Pylide-2=Ph_(3)P=CHMe and BHT=2,6-iBu_(2)-4-MeC_(6)H_(2)O) was demonstrated to be superior by which homopolymers PAMAs(M_(n)=27.6-111.5kg/mol and ■=1.14-1.25) and PVMAs(M_(n)=28.4-78.4 kg/mol and ■=1.12-1.18) and block copolymers PMMA-b-PAMA,PAMA-b-PVMA,PAMA-bPMMA,PMMA-b-PAMA-b-PMMA,PAMA-b-PMMA-b-PAMA,and PAMA-b-PVMA-b-PAMA were *** the polymerizations,all of the monomers were reacted by the conjugated ester vinyl groups leaving intactly the nonconjugated acryloxy *** pendant acryloxy groups attached to the main chain enable further to post-functionalization by the AIBN-induced radical "thiol-ene" reaction using PhCH_(2)*** thiolether side group-containing polymers PAMA-SCH_(2)Ph and PAMA-SCH_(2)Ph-b-PMMA-b-PAMA-SCH_(2)Ph were thus prepared.

关键词： Phosphonium ylide Alkenyl methacrylate Chemoselectivity Living/controlled polymerization Post-functionalization

Metal-metal bonds in Zintl clusters:Synthesis,structure and bonding in[Fe_(2)Sn_(4)Bi_(8)]^(3-)and[Cr_(2)Sb_(12)]^(3-)

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Chinese Chemical Letters 2024年第8期35卷 558-566页

作者： Ya-Nan Yang Zi-Sheng Li Sourav Mondal Lei Qiao Cui-Cui Wang Wen-Juan Tian Zhong-Ming Sun John E.McGrady state key laboratory of Element-organic chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of chemistry University of OxfordInorganic Chemistry LaboratoryOxfordOX13QRUnited Kingdom

We report here the synthesis and characterization of two new members of the M2 E 12 family of endohe-dral Zintl clusters,[Fe_(2)Sn_(4)Bi_(8)]^(3-)and[Cr_(2)Sb_(12)]^(3-),both of which contain open-shell metal dimers encap-sulated inside a triple-decker cluster of main-group *** 75-electron[Fe_(2)Sn_(4)Bi_(8)]^(3-)cluster has a D4h-symmetric structure,while[Cr_(2)Sb_(12)]^(3-),despite having the same 75-electron count,is strongly dis-torted to a geometry that resembles a CrSb_(8)crown capped by a CrSb_(4)*** structural differences between the two are driven by the increasing availability of 3d electron density in the earlier transi-tion metal,which leads,ultimately,to different electronic configurations in the two *** trends precisely mirror those observed in the ME_(10)and ME_(12)families containing a single transition metal ion.

关键词： Zintl anions Endohedral clusters Metal-metal bond Second-order Jahn-Teller effect DFT calculation

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

Recent progress on the functionalization of white phosphorus in China

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National Science Review 2024年第6期11卷 308-320页

作者： Xinlei Huangfu Zhongzhen Wang Yu Chen Junnian Wei Wei Liu Wen-Xiong Zhang Beijing National laboratory for Molecular Sciences(BNLMS) State Key Laboratory of Rare-Earth Materials Chemistry and Applications & Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University

Direct synthesis of organophosphorus compounds from white phosphorus represents a significant but challenging subject, especially in the context of ongoing efforts to comprehensively improve the phosphorus-derived chemical industry driven by sustainability and safety concerns. China is the world's largest producer of white phosphorus, creating a significant demand for the green transformation of this crucial feedstock. This review provides an overview of advancements in white phosphorus activation by Chinese research teams, focusing on the direct construction of P–C/N/O/S/M bonds from white phosphorus. Additionally, we offer some insights into prospective directions for the activation and transformation of white phosphorus in the future. This review paper aims to attract more researchers to engage in this area, stimulating follow-up exploration and fostering enduring advances.

关键词： white phosphorus organophosphorus compound activation selectivity efficiency

Nitrogen and fluorine co-doped graphene for ultra-stable lithium metal anodes

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Nano Research 2024年第8期17卷 7212-7220页

作者： Pan Li Yifan Liu Xujian Bao Jinghao Xie Zhao Li Hongcheng Li Qiang Ren Xiaomiao Feng Yue Hu Yanwen Ma state key laboratory for organic Electronics and Information Displays(KLOEID)and Jiangsu key laboratory for biosensors Institute of Advanced Materials(IAM)Nanjing University of Posts and TelecommunicationsNanjing 210023China key laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325000China

The heteroatom doping strategies have been utilized to effectively improve the performance of the carbon-based hosts,such as graphene,for lithium(Li)metal in high energy density lithium metal ***,solely doped graphene hosts often need the assistance of other materials with either better lithiophilicity or electronic conductance to achieve smooth and efficient deposition of Li,which adds extra weight or ***,graphene co-doped by nitrogen and fluorine(NFG)is employed as a stable host for Li,where the N-doping provides lithiophilicity and electronic conductivity lacked by F-doping and the F-doping facilitates fast formation of solid electrolyte interphase(SEI)retarded by *** well regulation of Li plating/stripping and SEI formation is verified by quickly stabilized and small-magnitude voltage hysteresis,which stands out in Li hosts based on doped graphene and leads to excellent long-term cycling performance of NFG based electrodes.A voltage hysteresis of 20 mV is observed for more than 850 h in the symmetrical *** remarkable efficiency of lithium usage is confirmed by the highcapacity retention of a full cell paired with LiFePO_(4)(LFP),which exceeds 70%after 500 *** work presents an innovative perspective on the control of Li plating/stripping by simultaneously introducing two kinds of dopants into graphene and paving the way for exploring practical Li metal batteries.

关键词： Co-doped graphene lithium metal anode dendrite suppression lithiophilic skeleton solid electrolyte interphase(SEI)formation

Antimony doped CsPbI_(2)Br for high-stability all-inorganic perovskite solar cells

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Nano Research 2024年第3期17卷 1508-1515页

作者： Mengfei Zhu Lina Qin Yuren Xia Junchuan Liang Yaoda Wang Daocheng Hong Yuxi Tian Zuoxiu Tie Zhong Jin state key laboratory of Coordination chemistry Ministry of Education(MOE)Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Nanjing Tieming Energy Technology Co. Ltd.Nanjing 210093China Suzhou Tierui New Energy Technology Co. Ltd.Suzhou 215228China

All-inorganic perovskites,adopting cesium(Cs+)cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites,have attracted much attention owing to the excellent thermal ***,all-inorganic iodine-based perovskites generally exhibit poor phase stability in ambient ***,we propose an efficient strategy to introduce antimony(Sb^(3+))into the crystalline lattices of CsPbI_(2)Br perovskite,which can effectively regulate the growth of perovskite crystals to obtain a more stable perovskite *** to the much smaller ionic radius and lower electronegativity of trivalent Sb^(3+)than those of Pb^(2+),the Sb^(3+)doping can decrease surface defects and suppress charge recombination,resulting in longer carrier lifetime and negligible *** a result,the all-inorganic perovskite solar cells(PSCs)based on 0.25%Sb^(3+)doped CsPbI_(2)Br light absorber and screen-printable nanocarbon counter electrode achieved a power conversion efficiency of 11.06%,which is 16%higher than that of the control devices without Sb^(3+)***,the Sb^(3+)doped all-inorganic PSCs also exhibited greatly improved endurance against heat and *** to the use of low-cost and easy-to-process nanocarbon counter electrodes,the manufacturing process of the all-inorganic PSCs is very convenient and highly repeatable,and the manufacturing cost can be greatly *** work offers a promising approach to constructing high-stability all-inorganic PSCs by introducing appropriate lattice doping.

关键词： all-inorganic perovskite solar cells Sb doped cesium lead halide perovskites foreign B-site ions hole-conductor-free phase stability improvement

Dimensional reduction enhances photocatalytic carbon dioxide reduction performance of metal-organic frameworks

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Nano Research 2024年第5期17卷 3653-3659页

作者： Kaiyue Ma Jixin Li Jinlu Liu Chunguang Li Zhan Shi Shouhua Feng state key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)have shown significant potential as *** has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be *** this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the ***(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,*** CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of *** result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb *** study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.

关键词： photocatalysis CO_(2)reduction metal-organic frameworks(MOFs) nanosheets light absorption

Promising thermal photonic management materials for sustainable human habitat

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Nano Research 2024年第1期17卷 112-131页

作者： Houze Yao Qihua Liao Huhu Cheng Liangti Qu key laboratory of organic Optoelectronics&Molecular Engineering Ministry of EducationDepartment of ChemistryLaboratory of Flexible Electronics TechnologyTsinghua UniversityBeijing 100084China state key laboratory of Tribology in Advanced Equipment(SKLT) Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China

The spectral characteristics of outdoor structures,such as automobiles,buildings,and clothing,determine their energy interaction with the environment,from broad-spectrum absorption of light energy to high-efficiency thermal *** developed spectrally selective absorption(SSA)materials permit the reduction of energy loss from human habitat eco-system in the sustainable way and further reduce the utilization of fossil energy to achieve carbon *** we review recent advances in SSA materials that enable rational and efficient management of thermal energy and provide new solutions for the resource base that supports human life like comfortable heat management,electricity production,and water *** basic principles of thermal photonic management,the regulation of SSA materials,and functional properties are *** outlook discussing challenges and opportunities in SSA material energy management for comfortable living environments is finally presented,which expects the enormous potential of this interdisciplinary research in solving growing resource-shortage of human society.

关键词： spectrally selective absorption passive cooling solar power eco-system