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CoTCPP integrates with BiOBr microspheres for improved solar-driven CO_(2)reduction performance

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Green Energy & Environment 2025年第1期10卷 193-202页

作者： Lina Li Yi Zhang Gaopeng Liu Tiange Wei Junze Zhao Bin Wang Mengxia Ji Yuanbin She Jiexiang Xia Huaming Li School of chemistry and Chemical Engineering Institute for Energy ResearchJiangsu University301 Xuefu RoadZhenjiang212013China State Key Laboratory Breeding Base of Green chemistry-Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou310014China

CO_(2) photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse ***,the 5,10,15,20-tetra(4-carboxyphenyl)porphyrin cobalt(II)(CoTCPP)has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr *** as-prepared CoTCPP/BiOBr-2 composite shows optimized photocatalytic performance for CO_(2) conversion into CO and CH_(4) upon irradiation with 300 W Xe lamp,which is 2.03 and 2.58 times compared to that of BiOBr,*** introduced CoTCPP significantly enhanced light absorption properties,promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO_(2) *** metal Co^(2+) at the center of the porphyrin molecules also acts as adsorption center for CO_(2) molecules,accelerating the CO_(2) conversion into CO and CH_(4).The possible mechanism of CO_(2) photoreduction was explored by in-situ FT-IR *** work offers a new possibility for the preparation of advanced photocatalysts.

关键词： BiOBr CoTCPP CO_(2)photoreduction Carriers transfer CO_(2)adsorption-activation

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Folding encapsulation toward Lindqvist polyoxometalates within adaptive coordination cages for catalysis

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Science China chemistry 2025年第2期68卷 561-569页

作者： Ying-Mei Zhong Jin-Jin Xuan Xujie Qin Han Xiao Zi-Jun Xia Li-Peng Zhou Xiao-Qing Guo Yu-Hang Hu Lu Zhang Chunsen Li Li-Xuan Cai Qing-Fu Sun State Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China College of chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China

In nature,enzymes at specific folded conformations exhibit high substrate complementarity,enabling them to efficiently and selectively catalyze biochemical *** by enzymes,coordination cages with conformational dynamics have been designed and are receiving increasing attention due to their versatile applications in allosteric guest binding and *** present here two enzyme-mimicking adaptive macrocycle-based coordination cages,Pd_(2)L_(2)^(1) and Pd_(2)L_(2)^(2),from macrocycle-based ligands(L^(1) and L^(2))and the encapsulation and stabilization of Lindqvist polyoxometalates anions M6O192−(M=W or Mo)in neutral aqueous solution.X-ray crystallographic studies have verified the formation of 1:1 host-guest complexes of two Pd_(2)L_(2) cages and the W6O192−anion,via an induced-fit folding *** with the free host,Pd_(2)L_(2)^(1) exhibited an induced-fit semi-folded conformation in the inclusion complex,while Pd_(2)L_(2)^(2) adopted an induced-fit fully-folded ***,the Mo_(6)O_(19)⊂Pd_(2)L_(2) host-guest complexes demonstrate high yield and selectivity in the oxidative decontamination reaction of the sulfur mustard simulant,2-chloroethyl ethyl *** work not only sheds light on the importance of conformational adaptability in enzyme-like systems but also paves the way for protecting labile POM clusters via host-guest encapsulation toward enhanced catalytic performance in aqueous solution.

关键词： coordination cage induced-fit polyoxometalates host-guest chemistry supramolecular catalysis

Sequence-activated chemiluminescence probes:programmable illumination for high-contrast in vivo sensing and imaging

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Science China chemistry 2025年第1期68卷 26-34页

作者： Yutao Zhang Juan Li Wei-Hong Zhu Zhiqian Guo Shanghai Key Laboratory of Functional Materials chemistry Joint International Research Laboratory of Precision Chemistry and Molecular EngineeringInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Bioreactor Engineering Shanghai Frontier Science Research Base of Optogenetic Techniques for Cell MetabolismEast China University of Science&TechnologyShanghai 200237China

Sequence-activated chemiluminescence(CL)technique offers a unique approach to detecting specific biomolecules or cellular events with high sensitivity and spatial *** fundamental principle behind sequence-activated CL probes involves tailoring highly-controllable CL signals in response to specific sequences or events of interest,thus enabling high-contrast signals under complex physiological *** sequential activation could be triggered by enzymes,reactive oxygen species(ROS),biothiols or changes in the *** unique sequence-activated CL probes bestow several advantages,including minimal background,deep-tissue penetration,and the ability of non-invasive or minimally invasive *** sequence-activated CL techniques represent a significant advancement in molecular imaging and *** this mini-review,we focus on the latest developments in sequential CL probes,addressing the technical challenges and discussing the future trajectory by harnessing CL signaling and molecular recognition.

关键词： chemiluminescnece sequence-activation in-vivo bioimaging cyclic peroxide

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Design of multifunctional interfaces on ceramic solid electrolytes for high-performance lithium-air batteries

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Green Energy & Environment 2025年第1期10卷 183-192页

作者： Yunxin Shi Ziyang Guo Changhong Wang Mingze Gao Xiaoting Lin Hui Duan Yonggang Wang Xueliang Sun College of Energy Material and chemistry College of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot010021China Department of Mechanical and Materials Engineering Western UniversityLondonONN6A 5B9Canada Department of chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghai200433China Eastern Institute for Advanced Study Eastern Institute of TechnologyNingboZhejiang315100China

High-energy-density lithium(Li)–air cells have been considered a promising energy-storage system,but the liquid electrolyte-related safety and side-reaction problems seriously hinder their *** address these above issues,solid-state Li–air batteries have been widely ***,many commonly-used solid electrolytes generally face huge interface impedance inLi–air cells and also showpoor stability towards ambient air/Li ***,we fabricate a differentiating surface-regulated ceramic-based composite electrolyte(DSCCE)by constructing disparately LiI-containing polymethyl methacrylate(PMMA)coating and Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)layer on both sides of Li_(1.5)Al_(0.5)Ge_(1.5)(PO_(4))_(3)(LAGP).The cathode-friendly LiI/PMMA layer displays excellent stability towards superoxide intermediates and also greatly reduces the decomposition voltage of discharge products in Li–air ***,the anode-friendly PVDF-HFP coating shows low-resistance properties towards ***,Li dendrite/passivation derived from liquid electrolyte-induced side reactions and air/I-attacking can be obviously suppressed by the uniformand compact composite *** a result,the DSCCE-based Li–air batteries possess high capacity/low voltage polarization(11,836mAh g^(-1)/1.45Vunder 500mAg^(-1)),good rate performance(capacity ratio under 1000mAg^(-1)/250mAg^(-1) is 68.2%)and longterm stable cell operation(~300 cycles at 750 mA g^(-1) with 750 mAh g^(-1))in ambient air.

关键词： Li-air batteries Li_(1.5)Al_(0.5)Ge_(1.5)(PO_(4))_(3) Polymers Composite electrolyte Ambient air

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Elucidating oxygen evolution and reduction mechanisms in nitrogen-doped carbon-based photocatalysts

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Chinese Chemical Letters 2025年第2期36卷 224-229页

作者： Yan Wang Jiaqi Zhang Xiaofeng Wu Sibo Wang Masakazu Anpo Yuanxing Fang State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University Sino-UK International Joint Laboratory on Photocatalysis for Clean Energy and Advanced Chemicals & Materials Fuzhou University Department of chemistry and Materials Innovation Factory University of Liverpool

Solar-induced water oxidation reaction（WOR） for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages. WOR is also associated with important reduction reactions, such as oxygen reduction reaction（ORR）, which leads to the production of hydrogen peroxide（H2O2）. These transitions are instrumental in the emergence and evolution of life. In this study, transition metals were loaded onto nitrogen-doped carbon（NDC） prepared under the primitive Earth's atmospheric conditions. These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination. The chemical pathways initiated by the pristine and metal-loaded NDC were investigated. This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.

关键词： Chemical vapor deposition Nitrogen-doped carbon Oxygen reduction reaction Photocatalysis Water oxidation reaction

Unraveling the potential-dependent degradation mechanism in Fe–N–C catalysts for oxygen reduction reaction

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Science China chemistry 2025年第04期 1541-1549页

作者： Yuyi Chu Yuqing Cheng Pengbo Wang Jingsen Bai Xin Guan Shuo Wang Chang Lan Hongxiang Wu Zhaoping Shi Siyuan Zhu Wei Liu Changpeng Liu Meiling Xiao Wei Xing State Key Laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences

Fe–N–C is hailed as the most promising candidate for replacing costly platinum-based catalysts for proton-exchange membrane fuel cells(PEMFCs) owing to their impressive catalytic activity and low cost. However, the durability of Fe–N–C catalysts remains a major challenge, primarily due to an insufficient understanding of their degradation mechanisms. In this study, we monitor the real-time changes in the electrode during the oxygen reduction reaction(ORR), shedding light on the potentialdependent degradation mechanisms inherent to Fe–N–C catalysts. Utilizing in-situ differential electrochemical mass spectroscopy, we identify three distinct potential regions with varying degrees of performance loss, notably observing carbon corrosion signals at low potentials. Theoretical calculations and fluorescence probe experiments corroborate that degradation mechanisms at high potentials are primarily driven by strong oxidative potentials that overcome the carbon oxidation energy barrier, whereas the degradation at low potentials is predominantly caused by the high concentrations of reactive oxygen species(ROS) generated during the ORR. The potential-dependent carbon corrosion consequently leads to a similar dependence of demetallation of active sites on the working potential. This study offers a comprehensive understanding of the intrinsic interrelations among various degradation mechanisms, thus paving the way for enhancing the durability of Fe–N–C catalysts in PEMFC applications.

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Recycling Fe and improving organic pollutant removal via in situ forming magnetic core-shell Fe_(3)O_(4)@CaFe-LDH in Fe(Ⅱ)-catalyzed oxidative wastewater treatment

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Journal of Environmental Sciences 2025年第1期147卷 523-537页

作者： Ting He Jie Sun Liangwei Deng Jialin Ming Changwei Hu Key Laboratory of Green chemistry and Technology Ministry of EducationCollege of ChemistrySichuan UniversityChengdu 610064China Biogas Institute of Ministry of Agriculture and Rural Affairs Chengdu 610041China Inner Mongolia Key Laboratory of Fine Organic Synthesis Inner Mongolia UniversityHohhot 010021China

Due to its high efficiency,Fe(Ⅱ)-based catalytic oxidation has been one of the most popular types of technology for treating growing organic pollutants.A lot of chemical Fe sludge alongwith various refractory pollutantswas concomitantly produced,whichmay cause secondary environmental problemswithout proper *** here innovatively proposed an effective method of achieving zero Fe sludge,reusing Fe resources(Fe recovery=100%)and advancing organics removal(final TOC removal>70%)simultaneously,based on the in situ formation of magnetic Ca-Fe layered double hydroxide(Fe_(3)O_(4)@CaFe-LDH)***(Ca^(2+)and Fe^(3+))concentration(≥30 mmol/L)and their molar ratio(Ca:Fe≥1.75)were crucial to the success of the *** nano Fe_(3)O_(4)was designed to be involved in the Fe(Ⅱ)-catalytic wastewater treatment process,and was modified by oxidation intermediates/products(especially those with COO-structure),which promoted the co-precipitation of Ca^(2+)(originated from Ca(OH)_(2)added after oxidation process)and byproduced Fe^(3+)cations on its surface to in situ generate core-shell Fe_(3)O_(4)@*** oxidation products were further removed during Fe_(3)O_(4)@CaFe-LDH material formation via intercalation and *** applicable to many kinds of organicwastewater,such as bisphenol A,methyl orange,humics,and biogas *** prepared magnetic and hierarchical CaFe-LDH nanocomposite material showed comparable application performance to the recently reported *** work provides a new strategy for efficiently enhancing the efficiency and economy of Fe(Ⅱ)-catalyzed oxidative wastewater treatment by producing high value-added LDHs materials.

关键词： CaFe layered double hydroxide Fe(Ⅱ)-catalytic oxidation Fe recycling Magnetic nanomaterial in situ formation Fe_(3)O_(4)modification

ZIF-90-loaded DNAzyme-responsive PROTAC for the self-powered degradation of NF-κB

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Science China chemistry 2025年第2期68卷 687-693页

作者： Min Hou Liang Sun Tianyu Ren Mingda Li Chao Hu Rong Liu Shuang Gu Mingyan Jiang Jian-Hui Jiang Jianjun He College of Physics and chemistry Hunan First Normal UniversityChangsha 410205China Hunan Provincial Key Laboratory of Animal Models and Molecular Medicine College of Biomedical SciencesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Xiangtan Central Hospital Xiangtan 411199China

Transcription factors(TFs)play vital roles in regulating gene *** or mutated TFs are implicated in a wide array of diseases,highlighting their potential as drug ***,TFs are considered undruggable by conventional inhibitor-based *** recently emerged proteolysis targeting chimeras(PROTACs)have exhibited great potential in tackling *** particular,DNA-ligand chimeras that arm E3 ligase-recruiting ligands to TF-binding double-strand DNA represent a promising strategy for the targeted proteolysis of ***,we report a DNAzyme-inducible PROTAC(DzTAC)that selectively degrades NF-κB in a zinc ion-dependent *** further applied zinc-imidazolate metal–organic framework90(ZIF-90)to encapsulate DzTAC(ZIF-90@DzTAC),facilitating its delivery into cancer cells while self-supplying Zn2+via adenosine triphosphate(ATP)-triggered ZIF-90 ***,ZIF-90@DzTAC can enhance the treatment efficacy of doxorubicin-based chemotherapy in tumor-bearing *** developed DzTAC provides specific modulation over TF activity and opens an avenue for more functional nucleic acid-based control over targeted protein degradation.

关键词： inducible proteolysis DNAzyme transcription factor ZIF-90 NF-κB

Stepwise assembly to construct stable copper(I) cluster-based circularly polarized luminescent MOFs

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Science China chemistry 2025年

作者： Jing-Wen Xie Meng-Ting Wang Yan Jin Si Li Jian-Hua Qin Shuang-Quan Zang Tomas C.W.Mak College of chemistry Henan Key Laboratory of Crystalline Molecular Functional Materials Zhengzhou University College of chemistry and Chemical Engineering Luoyang Normal University Department of chemistry The Chinese University of Hong Kong

Circularly polarized luminescence （CPL） materials have been extensively studied in recent years owing to their widespread applications in 3D display,optical storage,optical anti-counterfeiting,and biological imaging,***（I） clusters have emerged as a promising candidate for CPL materials,driven by their cost-effectiveness,superior luminescent properties,precise structure,and low ***,the poor environmental stability of copper（I） clusters renders their synthesis and preservation challenging,thereby significantly impeding their ***,we have designed and synthesised a chiral double-coordinated ligand in order to construct copper（I） cluster nodes that can be further *** anticipated,by utilizing stepwise assembly strategy,a Cu4cluster node co-modified by chiral alkynyl ligands and triphenylphosphine was further assembled with Cd2+ions to obtain 2D layers structure,L/*** L/D-Cu4-Cd exhibits excellent stability and optical properties,including bright yellow emission,solvent-responsive luminescence,and CPL activity with a maximum glumup to 2.0×10-3,which shows potential applications in the WLED and *** interestingly,the material also exhibits deflection ability towards different wavelengths of linearly polarized light,showing certain potential in the preparation of circular polarizer.

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