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Chinese chemical Letters 2025年第2期36卷 189-194页

作者： Gang Hu Chun Wang Qinqin Wang Mingyuan Zhu Lihua Kang School of chemistry and chemical engineering/State Key Laboratory Incubation Base for Green Processing of chemical engineering Shihezi University College of chemistry&chemical engineering Yantai University

In this paper,low-temperature dielectric-blocked discharge plasma （DBD） was employed for the first time to treat silica-doped H4PMo11VO40（HPAV） catalysts (DBD（Ar/x）-MF-Catal) and apply them in the catalytic methacrolein （MAL） selective oxidation to produce methacrylic acid （MAA）.This work investigates in detail the controllable regulation of the concentration of oxidation states on silica-doped HPAV catalysts by adjusting the DBD discharge with controlled changes in voltage,current,treatment time,and treatment *** reports the intrinsic correlation between oxidation states and MAL oxidation *** research results indicated that the catalytic performance was related to the presence of oxygen vacancies and oxygen species (VO2+),and are the main reason for the selective oxidation of MAL to ***,the generation of oxygen vacancies and VO2+altered localized electrons,which resulted in the easier activation of *** calculations of DFT also proved the formation mechanism of oxygen vacancies and VO2+and electron properties on high-performance polymers,which elucidated the intrinsic influence of catalyst *** DBD（Ar/10）-MF-Catal catalysts with suitable VO2+and oxygen vacancy concentrations exhibited the highest catalytic performance with 90%MAL conversion and 70%MAA selectivity and showed good stability （500 h）.

关键词： Catalyst Dopant Methacrolein Methacrylic acid Oxygen vacancy Plasma

Synthesis of ternary geopolymers using prediction for effective solidification of mercury in tailings

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Journal of Environmental Sciences 2025年第1期147卷 392-403页

作者： Xuan Lu Jinfa Guo Fang Chen Mengkui Tian School of chemistry and chemical engineering Guizhou UniversityGuiyang 550025China

This study used steel slag,fly ash,and metakaolin as raw materials(SFM materials)to create silica-alumina-based geopolymers that can solidify Hg^(2+)when activated with sodiumbased water *** experiments began with a triangular lattice point mixing design experiment,and the results were fitted,analyzed,and *** optimum SFM material mass ratio was found to be 70%steel slag,25%fly ash,and 5%*** optimum modulus of the activator was identified by comparing the unconfined compressive strength and solidifying impact on Hg^(2+)of geosynthetics with different *** SFM geopolymer was then applied in the form of potting to cure the granulated mercury *** inclusion of 50%SFM material generated a geosynthetic that reduced mercury transport to the surface soil by roughly 90%.The mercury concentration of herbaceous plant samples was also reduced by 78%.It indicates that the SFM material can effectively attenuate the migration transformation of ***,characterization methods such as XPS and FTIR were used to investigate the mechanism of Hg^(2+)solidification by geopolymers generated by SFM *** possible solidification mechanisms were proposed as alkaline environment-induced mercury precipitation,chemical bonding s,surface adsorption of Hg^(2+)and its precipitates by the geopolymer,and physical encapsulation.

关键词： Mercury Geopolymer Solidification Tailings

Three-in-one erlotinib-modified NIR photosensitizer for fluorescence imaging and synergistic chemo-photodynamic therapy

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Chinese chemical Letters 2025年第2期36卷 323-327页

作者： Du Liu Yuyan Li Hankun Zhang Benhua Wang Chaoyi Yao Minhuan Lan Zhanhong Yang Xiangzhi Song College of chemistry & chemical engineering Central South University

Photodynamic therapy(PDT) presents a promising avenue in cancer treatment. Erlotinib, an FDAapproved anticancer drug targeting epidermal growth factor receptor(EGFR), has shown effectiveness in normalizing tumor vasculature across various tumors, thereby promoting tumor oxygenation and facilitating PDT. In this work, erlotinib was conjugated with a near-infrared(NIR) photosensitizer,benzo[a]phenoselenazinium, yielding three EGFR-targeted PDT agents(NBSe-n C-Er). These newly synthesized photosensitizers demonstrate specificity in binding to EGFR, thereby enhancing their accumulation in cancer cells and tumors, and consequently improving the efficiency of both PDT and ***, the NIR fluorescence emitted by the photosensitizer allows for imaging-guided therapy, offering a non-invasive means of monitoring treatment progress. The distinctive properties of the three-inone photosensitizer render it an ideal candidate for precise tumor treatment, overcoming the limitations of conventional therapies.

关键词： Benzo[a]phenoselenazinium Chemotherapy Fluorescence imaging Photodynamic therapy Photosensitizer

Polyvinyl alcohol fiber with enhanced strength and modulus and intense cyan fluorescence based on covalently functionalized graphene quantum dots

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Chinese chemical Letters 2025年第2期36卷 250-255页

作者： Manman Ou Yunjian Zhu Jiahao Liu Zhaoxuan Liu Jianjun Wang Jun Sun Chuanxiang Qin Lixing Dai College of chemistry Chemical Engineering and Materials Science Soochow University

In this study, we proposed a novel and efficient way to strengthen polyvinyl alcohol(PVA) fiber using graphene quantum dots(GQDs). PVA molecular chains were grafted onto the surface of GQDs through Friedel-Crafts alkylation reaction to obtain functionalized GQDs(f-GQDs), and PVA/f-GQDs composite fiber was successfully prepared by wet spinning and post-treatment. The tensile strength and Young's modulus of the composite fiber reached up to 1229.24 MPa and 35.36 GPa which were approximately twice and 4 times those of the pure PVA fiber, respectively. Moreover, the composite fiber was demonstrated excellent resistance to solvents. In addition, the PVA/f-GQDs composite fiber showed intense and uniform cyan fluorescence, meanwhile, it could maintain stable solid-state fluorescence in acid and alkali solutions and particularly after long-term immersion in water(1 month). This study proposes a promising route for obtaining high-performance conventional fibers with some new functions.

关键词： Enhancement Fluorescence Graphene quantum dots Polyvinyl alcohol fiber

CaH2-promoted activity of Ni-carbonate interface for CO_(2) methanation

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Journal of Energy chemistry 2025年第1期100卷 522-532页

作者： Jin-Peng Wang Guo-Cui Mao Hui-Lin Jiang Bao-Xia Dong Yun-Lei Teng School of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002JiangsuChina

Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic *** interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)***,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)*** work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the *** CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) ***,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 *** research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)***_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H****,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.

关键词： CO_(2)methanation Metal hydride Ni catalysts Carbonate Metal-carbonate interface

Dual modulation of homogeneous nanomaterialization and electrochemical activation enhancing zinc ion storage

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Science China chemistry 2025年第1期68卷 385-393页

作者： Jianwei Wang Huan Wang Kangning Wang Wenhui Wang Wenlin Zhang Yanzhong Zhen School of chemistry&chemical engineering Yan’an UniversityYan’an 716000China

Vanadium-based electrode materials are widely investigated,but the low specific capacity and slow electrochemical kinetics in aqueous zinc-ion batteries still limit their commercial ***,the VS_(2)/Ca V_(4)O_(9)material with the morphology of nanoflower was synthesized by a one-step hydrothermal *** to the blocky structure of pure VS_(2)material,the VS_(2)/Ca V_(4)O_(9)material is composed of thinner homogeneous *** open structures could provide abundant electrochemical active sites and ion transport channels,and then promote the electrochemical reaction *** addition,they can also buffer the bulk strain during the reaction *** improve the utilization of vanadium elements,an in-situ electrochemical activation strategy is used to explore the storage performance of the VS_(2)/Ca V_(4)O_(9)material,the different activation voltage range of 0.4–1.6 and 0.4–1.4 V are selected,*** with the longer activation plateau of activated-VS_(2),the VS_(2)/Ca V_(4)O_(9)cathode could quickly reach the activation state in the range of 1.4–1.6 V and cause the release of additional Zn storage sites *** VS_(2)/Ca V_(4)O_(9)cathode delivers a higher power density of 37,000 W kg^(-1)and a significant energy density of 423 Wh kg^(-1).At the high current density of 15 A g^(-1),the VS_(2)/Ca V_(4)O_(9)cathode still has a discharge capacity of 183.9m Ah g^(-1)after 5,000 cycles,and the capacity decay rate per cycle is only 0.0042%.Continuous cyclic voltammetry(CV)curves,electrochemical impedance spectroscopy(EIS)measurements,density functional theory(DFT)calculation and galvanostatic intermittent titration technique(GITT)measurements demonstrate that the VS_(2)/Ca V_(4)O_(9)cathode has a faster ion diffusion/charge transfer ***,the assembled flexible device has an excellent mechanical stability.

关键词： dual modulation homogeneous nanomaterialization electrochemical activation zinc ion storage

Molecular-based porous polymers with precise sites for photoreduction of carbon dioxide

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Chinese chemical Letters 2025年第1期36卷 201-213页

作者： Wei-Jia Wang Kaihong Chen College of Biological and chemical engineering Zhejiang University of Science and TechnologyHangzhou 310023China The Institute of Green chemistry and engineering School of Chemistry and Chemical EngineeringNanjing UniversitySuzhou 215163China

Photocatalytic CO_(2)reduction reaction(CO_(2)RR)is one of the promising strategies for sustainably producing solar *** precise identification of catalytic sites and the enhancement of photocatalytic CO_(2)conversion is imperative yet quite *** critical review summarizes recent advances in porous photo-responsive polymers,including covalent organic frameworks(COFs),covalent triazine frameworks(CTFs),and conjugated microporous polymers(CMPs),those can be rationally designed from the molecular level for visible-light-driven photocatalytic CO_(2)***,special emphasis is placed on how the well-defined active sites on these polymers can influence their properties and photocatalytic *** precise regulation and control of microenvironments and electronic properties of metal active centers are crucial for boosting catalytic efficiency and selectivity,as well as for the design of better photocatalysts for CO_(2)reduction.

关键词： Carbon dioxide reduction Photocatalysis Porous polymers Well-defined catalytic sites Molecular level

Deciphering the role of ultra-low-loaded rhodium in NiFe-MIL-53 for superior oxygen evolution reaction

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Journal of Energy chemistry 2025年第1期100卷 77-86页

作者： Jinzhi Jia Jinhua Zhang Kailu Guo Lanyue Zhang Gening Du Hao You Junfeng Huang Mudong Tu Hua Li Yong Peng Wei Dou Cailing Xu State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringSchool of Materials and EnergyLanzhou UniversityLanzhou 730000GansuChina College of chemistry and chemical engineering Luoyang Normal UniversityLuoyang 471934HenanChina

Designing highly active and stable electrocatalysts of oxygen evolution reaction(OER)is one of the crucial *** this study,a novel OER electrocatalyst,NiFe-MIL-53 modified with ultra-low rhodium(Rh@NiFe-MIL-53),is successfully prepared via the hydrothermal ***-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active *** importantly,the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe(OH)_(2)after doping Rh is beneficial for improving the electrochemical stability of the catalyst.X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@***,theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap,regulates the d-band center(εd),accelerates the charge transfer,and optimizes the adsorption behavior of oxygen-containing intermediates,thereby lowering the energy barrier of rate-determining ***,the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity(240 mV)with a small Tafel slope of 48.2 mV dec^(-1)and long-term durability(over1270 h at 10 m A cm^(-2)and 110 h at 200 mA cm^(-2)).This work presents a new perspective on designing highly efficient OER electrocatalysts.

关键词： NiFe-MIL-53 Rh Electrochemical reconstruction Catalytic mechanism Oxygen evolution reaction

Critical new insights into the interactions of hexafluoropropylene oxide-dimer acid(GenX or HFPO-DA)with albumin at molecular and cellular levels

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Journal of Environmental Sciences 2025年第3期149卷 88-98页

作者： Shi-Ya Peng Ya-Di Yang Rong Tian Naihao Lu Jiangxi Key Laboratory of Green chemistry College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022China

A key characteristic to be elucidated,to address the harmful health risks of environmental perfluorinated alkyl substances(PFAS),is their binding modes to serum albumin,the most abundant protein in *** oxide-dimer acid(GenX or HFPO-DA)is a new industrial replacement for the widespread linear long-chain ***,the detailed interaction of new-generation short-chain PFAS with albumin is still ***,the binding characteristics of bovine serum albumin(BSA)to GenX were explored at the molecular and cellular *** found that this branched short-chain GenX could bind to BSA with affinity lower than that of legacy linear long-chain perfluorooctanoic acid(PFOA).Site marker competitive study and molecular docking simulation revealed that GenX interacted with subdomain IIIA to form BSA-GenX *** with its weaker affinity to albumin protein,the cytotoxicity of branched short-chain GenX was less susceptible to BSA binding compared with that of the linear long-chain *** contrast to the significant effects of strong BSA-PFOA interaction,the weak affinity of BSA-GenX binding did not influence the structure of protein and the cytotoxicity of *** detailed characterization and direct comparisons of serum albumin interaction with new generation short-chain GenX will provide a better understanding for the toxicological properties of this new alternative.

关键词： GenX Protein binding Albumin Cytotoxicity Risk assessment

Enantioselective reductive conjugate alkenylation ofα,β-enones with keto alkenyl acetates by nickel catalysis

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Science China chemistry 2025年第1期68卷 157-162页

作者： Rong-De He Yun-Lei Luo Qiu-Quan Pan Qi-Wei Yao Xing-Zhong Shu State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China

Reactions involving alkenyl acetates offer cost-effective and environmentally friendly routes for alkene synthesis,yet their asymmetric variant remains ***,asymmetric conjugate alkenylation predominantly centered on nucleophilic addition using alkenyl–*** manuscript presents an asymmetric reductive conjugate alkenylation reaction involving alkenyl *** method facilitates the enantioselective addition of keto alkenyl groups toα,β-enones,resulting in the formation of unsaturated diketones—a class of useful structural motifs that are challenging to access *** use of electron-rich Pyroxy ligand is essential for achieving both high reaction efficiency and enantioselectivity.

关键词： nickel alkenylation asymmetric cross-coupling alkenes