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Nano Research 2024年第7期17卷 6087-6094页

作者： Mao Qian Yakun Tang Lang Liu Yue Zhang Xiaohui Li JiaJia Chen state key laboratory of chemistry and Utilization of Carbon Based Energy Resources Xinjiang UniversityUrumqi 830017China state key laboratory of physical chemistry of solid surfaces Xiamen UniversityXiamen 361005China

The diffusion and loss of lithium polysulfides(LiPSs)in lithium-sulfur batteries(LSBs)reduce the sulfur utilization rate and the catalytic conversion efficiency of sulfur species,resulting in early battery ***_(2)ZnTi_(3)O_(8)(LZTO),characterized by its stable spinel structure,exhibits high Li+conductivity and holds great potential as an effective adsorbent for *** study proposes a collaborative design concept of LZTO host–separator modifier,which offers a complementary and matching approach in the cathode side,effectively addressing the challenges associated with dissolution and inadequate conversion of *** functional theory(DFT)calculation substantiates the pronounced chemical affinity of LZTO towards *** importantly,the high efficiency ion transport channels are achieved in separator coating due to the presence of the LZTO ***,the catalytic efficacy of LZTO is validated through meticulous analysis of symmetric batteries and Tafel ***,the LZTO host–separator modifier-based cell displays satisfactory rate capability(1449 and 1166 mAh·g^(−1)at 0.1 and 0.5 C)and an impressively capacity(606 mAh·g^(−1)after 500 cycles at 1 C).The coordinated strategy of host–separator modifier is supposed to have wide applications in LSBs.

关键词： Li_(2)ZnTi_(3)O_(8) lithium-sulfur batteries host-separator modifier catalytic conversion diffusion and loss of LiPSs

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

Linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system

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Green Energy & Environment 2024年第1期9卷 104-113页

作者： Xinxin Li Linchuan Cong Haibo Lin Fangbing Liu Xiangxue Fu Hai-Chao Xu Nan Lin state key laboratory of Inorganic Synthesis and Preparative chemistry Jilin UniversityChangchun 130012JilinChina state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the ***,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedﬂow cell *** reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are *** the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efﬁciency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.

关键词： Multiple redox mediated system Linear paired electrolysis Furfural Furoic acid

Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu Bo Zhou Long-Wu Ye key laboratory for Chemical Biology of Fujian Province and state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes

Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： Chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

Switching on/off phosphorescent or non-radiative channels by aggregation-induced quantum interference

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Aggregate

Aggregate 2024年第1期5卷 175-184页

作者： Yi Kong Yu-Chen Wang Xunkun Huang WanZhen Liang Yi Zhao department of chemistry State Key Laboratory of Physical Chemistry of Solid SurfacesiChEMFujian Provincial Key Laboratory of Theoretical and Computational Chemistryand College of Chemistry and Chemical EngineeringXiamen UniversityXiamenPeople’s Republic of China

Pure organic materials with persistent and efficient room-temperature phosphorescence have recently aroused great research interest due to their vast potential in *** crucial design principle for such materials is to suppress as much as possible the non-radiative decay of the triplet exciton while maintaining a moderate phosphorescent radiative ***,molecular engineering often exhibits similar regulation trends for the two ***,we propose that the quantum interference caused by aggregation can be utilized to control the phosphorescent and non-radiative decay *** systematically analyze various constructive and destructive transition pathways in aggregates with different molecular packing types and establish clear relationships between the luminescence characters and the signs of the singlet and triplet excitonic *** is shown that the decay channels can be flexibly switched on or off by regulating the packing type and excitonic *** importantly,an enhanced phosphorescent decay and a completely suppressed non-radiative decay can be simultaneously realized in the aggregate packed with inversion *** work lays the theoretical foundation for future experimental realization of quantum interference effects in phosphorescence.

关键词： excitonic coupling intersystem crossing organic aggregates organic room temperature phosphorescence quantum interference

Engineering and dynamics of heterogeneous catalysts via metal single atoms as promoters/precursors

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Science China chemistry 2024年第8期67卷 2547-2565页

作者： Jiwei Li Junli Xu Jingyun Yang Zitao Duan Zhun Zhang Haifeng Xiong state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province Xiamen 361102China

Metal single-atom catalysts(SACs) have emerged as a focal point of research, captivating the scientific community due to their distinctive electronic properties and unparalleled catalytic prowess in the realm of heterogeneous catalysis. However, their significance transcends their role as mere active sites. Recent investigations have illuminated the multifaceted capabilities of metal single atoms as catalyst promoters and precursors, paving the way for the engineering of highly efficient heterogeneous catalysts. Single-atom promoters not only enhance the stabilization of active metals and tailor the support material, but regulate the reactive interfacial structure, eventually tuning the catalytic performance. Furthermore, SACs were also used as catalyst precursors to design new catalyst active sites. During the pretreatment or catalytic reaction, the structure of the metal single sites is changed significantly and transformed into the new and more active state, which improve the adsorption and reactive ability of reactants or intermediates. In this critical review, we comment the recent development of metal SACs used as catalyst promoters/precursors in engineering heterogeneous catalysts, including thermal catalysis and electrocatalysis. Furthermore, the dynamic evolution of the SACs during the pretreatment or catalytic reaction is also discussed. Finally, we provide our insight to potentially guide the future development on this emerging field.

关键词： single-atom catalysts single-atom promoter single-atom precursor dynamic evolution

Screening of transition metal oxides for electrocatalytic nitrate reduction to ammonia at large currents

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Nano Research 2024年第5期17卷 3902-3910页

作者： Qiongfei Wu Weijie Zhu Dongxu Ma Chao Liang Zhoucheng Wang Hanfeng Liang state key laboratory of physical chemistry of solid surfaces Tan Kah Kee Innovation LaboratoryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemical Engineering Tianjin UniversityTianjin 300072China

Electrochemical nitrate reduction reaction(NO_(3)RR)towards ammonia,as an emerging and appealing technology alternative to the energy-intensive Haber-Bosch process and inefficient nitrogen reduction reaction,has recently aroused wide concern and ***,the current research of the NO_(3)RR towards ammonia lacks the overall performance comparison of various *** this,we here make a comparison of 12 common transition metal oxide catalysts for the NO_(3)RR under a high cathodic current density of 0.25 A·cm^(-2),wherein Co_(3)O_(4) catalyst displays the highest ammonia Faradaic efficiency(85.15%)and moderate activity(ca.-0.25 V *** hydrogen electrode).Other external factors,such as nitrate concentrations in the electrolyte and applied potential ranges,have also been specifically investigated for the NO_(3)RR.

关键词： nitrate reduction reaction ammonia production transition metal oxides Co_(3)O_(4)

Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Centre of chemistry for Energy Materials state key laboratory of physical chemistry of solid surfaces and department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China College of Chemical Engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

Synthetic Studies toward Pseudolaric Acids:Radical Cyclization to Form Bridged Scaffold

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Chinese Journal of chemistry 2024年第15期42卷 1699-1705页

作者： Yujie Niu Minggui Lin Hao Cui Yanji Huang Yang Shen Yandong Zhang state key laboratoryof physical chemistry of solid surfaces Key Laboratory of Chemical Biology of Fujian ProvinceicHEMCollege of Chemistryand Chemical EngineeringXiamen UniversityXiamenFujian 361005China

Pseudolaric acids are a family of diterpenoid natural products that exhibit a broad spectrum of biological *** main structural feature of their framework is a trans-fused perhydroazulene bearing a bridged lactone positioned at the junction of the ***,we have developed a radical cyclization strategy that allows flexible tuning of the cyclization process through diverse silicon substitutions on the *** strategy can assist in constructing a series of skeletons with structural resemblance to pseudolaric acids and expedites the construction of the bridged ***,it facilitates the synthesis of the entire skeletal structure of the pseudolaric acidfamily of natural products,excludingthe B-ringfunctionalization.

关键词： Terpenoids Total synthesis Radical cyclization Bridged cycles Regioselectivity