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Self-sustainable Catalytic Nucleic Acid Circuit Powered Hybrid CRISPR-Cas Systems for Point-of-Care Diagnosis of Circadian Clock Gene from Cell Lysates

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Journal of Analysis and Testing 2025年第01期 1-11页

作者： Zhiyuan Feng Ran Liu Enming Yang Rui Lian Jingjing Zhang State Key Laboratory of Analytical chemistry for Life Science School of Chemistry and Chemical Engineering Chemistry and Biomedicine Innovation Center (ChemBIC)Nanjing University

The CRISPR-Cas13 systems have opened a new avenue for RNA detection due to their exceptional programmable collateral activity against ssRNA. However, most high-performance Cas13-based RNA sensors still suffer from some drawbacks because of the tradeoffs between readout device complexity and analytical sensitivity, which can limit their viability at the point-of-care(POC). To overcome these shortcomings, we herein report a novel target-responsive POC platform for translating RNA detection into a glucose test. Specifically, this platform combines the advantages of three techniques: a hybrid Cas13a/Cas12a system for both RNA recognition with single-base resolution and cascade enzymatic amplification, a self-sustainable catalytic nucleic acid circuit(SCC) with embedded uracil-base and poly-T bulges for Cas13a-and Cas12amediated collateral cleavage, respectively, and a portable glucose meter(PGM) for simple signal readout. The incorporation of an engineered ssDNA–invertase conjugate in SCC led to RNA-to-glucose signal transduction through the hydrolysis of sucrose to glucose. By targeting a 20-nt conserved region of BMAL1 mRNA(mBMAL1), a key circadian clock gene, we demonstrate that SCC can serve as an excellent CRISPR reporter, enabling the direct detection of unamplified mBMAL1 as low as 0.864 fM concurrently with good discrimination ability for single-base mismatch. More importantly, this integrated platform was successfully applied for POC diagnosis of mBMAL1 from different cell lysates, with results that strongly correlate with RT-PCR. Given its wide adaptability, we anticipate that such a CRISPR-SCC system can be easily modified to quantify other RNA biomarkers associated with circadian rhythm.

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Depression mechanism of sulfite ions on sphalerite and Pb^(2+)activated sphalerite in the flotation separation of galena from sphalerite

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 335-345页

作者： Feng Zhang Chenyang Zhang Linlin Wu Wei Sun Hongliang Zhang Jianhua Chen Yong Pei Songjiang Li Engineering research center of Ministry of Education for Carbon Emission Reduction in Metal Resource Exploitation and Utilization Hunan International Joint Research Center for Efficient and Clean Utilization of Critical Metal Mineral ResourcesSchool of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083China State Key Laboratory of Mineral Processing Beijing General Research Institute of Mining&MetallurgyBeijing 100160China Hunan Provincial Key Laboratory of Micro&Nano Materials Interfaces Science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China School of Resources Environment and MaterialsGuangxi UniversityNanning 530004China Department of chemistry Xiangtan UniversityXiangtan 411105China China Railway Resource Group Co.Ltd Beijing 102300China

The depression mechanism of sulfite ions on sphalerite and Pb^(2+)activated sphalerite in the flotation separation of galena from sphalerite still lacked in-depth ***,the depression mechanism of sulfite ions on sphalerite and Pb^(2+)activated sphalerite in the flotation separation of galena from sphalerite was further systematically investigated with experiments and density functional theory(DFT)*** X-ray photoelectric spectroscopy(XPS)results,DFT calculation results,and frontier molecular orbital analysis indicated that sulfite ions were difficult to be adsorbed on sphalerite surface,suggesting that sulfite ions achieved depression effects on sphalerite through other non-adsorption ***,the oxygen content in the surface of sphalerite treated with sulfite ions in creased,which enhanced the hydrophilicity of the sphalerite and further increased the difference in hydrophilicity between sphalerite and ***,sulfite ions were chelated with lead ions to form PbSO_(3)in *** hydrophilic PbSO_(3)was more easily adsorbed on sphalerite than *** interaction between sulfite ions and lead ions could effectively inhibit the activation of *** addition the UV spectrum showed that after adding sulfite ions,the peak of perxanthate in the sphalerite treated xanthate solution was significantly stronger than that in the galena with xanthate solution,indicating that xanthate interacted more readily with sulfite ions and oxygen mo lecules within the sphalerite system,leading to the formation of ***,sulfite ions hardly depressed the flotation of ga lena and could promote the flotation of galena to some *** study deepened the understanding of the depression mechanism o sulfite ions on sphalerite and Pb^(2+)activated sphalerite.

关键词： sphalerite galena sulfite ion density functional theory depression mechanism

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Development of ESIPT-based specific fluorescent probes for bioactive species based on the protection-deprotection of the hydroxyl

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Chinese Chemical Letters 2025年第2期36卷 49-56页

作者： Haixian Ren Yuting Du Xiaojing Yang Fangjun Huo Le Zhang Caixia Yin Department of chemistry Xinzhou Normal University research Institute of Applied chemistry Shanxi University Department of chemistry The University of Texas at Austin Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Key Laboratory of Materials for Energy Conversion and Storage of Shanxi Province Institute of Molecular ScienceShanxi University

Excited-state intramolecular proton-transfer (ESIPT) based fluorescence probes are particularly attractive due to their unique properties including environmental sensitivity, a large Stokes shift, and potential for ratiometric sensing. In general, ESIPT-based fluorophore incorporates an intramolecular hydrogen bonding interaction between a hydrogen bond donor (–OH and NH2are common) and a hydrogen bond acceptor(C=N and C=O). More, protection–deprotection of hydroxyl group as hydrogen bond donor could induce an off-on switch of ESIPT-based emission. Therefore, protection–deprotection of hydroxyl group has been the widely used strategy to design fluorescent probes, where the potential key issue is selecting a protective group that can specifically leave in the presence of the target analyte. In this review, we mainly summarize the specific protecting groups (sites) and deprotection mechanisms for biologically important species (including reactive sulfur species (RSS), reactive oxygen species (ROS), enzymes, etc.), and analyze the advantages and disadvantages of different protection mechanisms from some aspects including probe stability, selectivity, response rate and assay system, etc. Based on the aforementioned, we further point out the current challenges and the potential future direction for developing ESIPT-based probes.

关键词： Bioimaging ESIPT Fluorescence probe Protection-deprotection Specificity

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Tunable Thermo-Responsive Shape Memory Materials Enabled by Poly(ε-caprolactone)-Poly(2-vinyl)ethylene Glycol Copolymers via Facile Thiol-Ene Photo-Crosslink

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Chinese Journal of Polymer Science 2025年第2期43卷 278-288页

作者： Ming-Hang Wang Fan Yang Yong-Jian Zhang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative Moleculesand School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai200240China Sichuan research Institute Shanghai Jiao Tong UniversityChengdu610042China

Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical *** this study,novel poly(ε-caprolactone)(PCL)-poly(2-vinyl)ethylene glycol(PVEG)copolymers bearing multi-pendant vinyl groups is synthesized by branched-selective allylic etherification polymerization of vinylethylene carbonate(VEC)with linear and tetra-arm PCLs under a synergistic catalysis of palladium complex and boron *** thiol-ene photo-click reaction of PCL-PVEG copolymers with multifunctional thiols can rapidly access a serious crosslinked SMPs with high shape memory *** thermal properties,mechanical properties and response temperature of the obtained SMPs are tunable by the variation of PCL prepolymers,vinyl contents and functionality of ***,high elastic modulus in the rubbery plateau region can be maintained effectively owing to high-density topological networks of the PCL *** addition,the utility of the present SMPs is further demonstrated by the post-functionalization via thiol-ene photo-click chemistry.

关键词： Shape memory polymers Polycaprolactone Thiol-ene photo-crosslink Controlled crosslinking density Tunable response temperature

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Deciphering Water Oxidation Catalysts:The Dominant Role of Surface chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi Zhichuan J.Xu Chun‑Hua Yan State Key Laboratory of Applied Organic chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key Laboratory of Baiyunobo Rare Earth Resource researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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Chiral phosphoramidite ligand-modulated palladium auto-tandem catalysis for asymmetric dehydrogenative dienylation of imines with α-alkenes

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Science China chemistry 2025年

作者： Zhong-Sheng Nong Hao-Fan Qian Ying-Chun Chen Pu-Sheng Wang Liu-Zhu Gong Hefei National research center for Physical Sciences at the Microscale and Department of chemistry University of Science and Technology of China Key Laboratory of Drug Targeting and Drug Delivery System (Sichuan University) Ministry of Education and Sichuan Research Center for Drug Precision Industrial Technology West China School of Pharmacy Sichuan University School of Materials and chemistry Southwest University of Science and Technology

The development of efficient processes allowing rapid access to complex chiral molecules from easily available alkenes is a long-term pursuit in the synthetic chemistry community. Transition metal-catalyzed asymmetric functionalization of allylic C–H bond represents a unique alternative toward this goal. However, enantioselective dehydrogenative transformation of olefins to value-added optically enriched molecules remains yet to be discovered. Here, we report a highly enantioselective dehydrogenative dienylation of imines with unactivated α-alkenes driven by the synergistic action of palladium complex and carboxylic acid. Chiral phosphoramidite ligands turned out to be superior in modulating the performance of palladium autotandem catalysis and allowed a broad range of α-alkenes and imines to be transformed into chiral dienylamines. Mechanistic studies suggest that the dienes could be in situ generated from α-alkenes through a palladium(0)-mediated dehydrogenative process in the presence of excess benzoquinone oxidants, and then participated in the Pd-chiral phosphoramidite-catalyzed intermolecular vinylogous-type addition to the imines activated by the carboxylic acid co-catalyst. Notably, the second β-H elimination occurring in the dienylation event might be the turnover-limiting step.

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A low redox potential and long life organic anode material for sodium-ion batteries

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Journal of Energy chemistry 2025年第1期100卷 557-564页

作者： Zhi Li Yang Wei Kang Zhou Xin Huang Xing Zhou Jie Xu Taoyi Kong Junwei Lucas Bao Xiaoli Dong Yonggang Wang Department of chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Institute of New EnergyCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)Fudan UniversityShanghai 200433China Department of chemistry Boston CollegeChestnut HillMA 02467USA School of Materials Science and Engineering Anhui University of TechnologyMa’anshan 243002AnhuiChina

Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ***,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials(>1 V).Organic electrodes with low redox potential that can be used as anode are ***,a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na_(4)TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic *** three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per ***,the Na_(4)TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm^(-2).By pairing with a thick Na_(3)V_(2)(PO_(4))_(3)cathode (20.6 mg cm^(-2)),the as-fabricated full cell exhibited high operating voltage (2.8 V),excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na_(4)TDC anode material for SIBs.

关键词： Organic anode material Low redox potential Composite anode Sodium-ion batteries

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A comparison increasing the photodegradation power of a Ag/g-C_(3)N_(4)/CoNi-LDH nanocomposite:Photocatalytic activity toward water treatment

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Journal of Environmental Sciences 2025年第2期148卷 437-450页

作者： Razieh Fazaeli Hamid Aliyan Darrin Richeson Yuning Li Department of Chemical Engineering Waterloo Institute for Nanotechnology(WIN)200 University Ave WWaterlooON N2L 3G1Canada Department of chemistry Shahreza BranchIslamic Azad University86145-311Iran Department of chemistry and Biomolecular Sciences Center for Catalysis Research and InnovationUniversity of OttawaOttawaOntarioK1N 6N5Canada

For environmental applications,it is crucial to rationally design and synthesize photocatalysts with positive exciton splitting and interfacial charge ***,a novel Agbridged dual Z-scheme Ag/g-C_(3)N_(4)/CoNi-LDH plasmonic heterojunction was successfully synthesized using a simple method,with the goal of overcoming the common drawbacks of traditional photocatalysts such as weak photoresponsivity,rapid combination of photogenerated carriers,and unstable *** materials were characterized by XRD,FT-IR,SEM,TEM UV-Vis/DRS,and XPS to verify the structure and stability of the *** pristine LDH,g-C_(3)N_(4),and Ag/g-C_(3)N_(4)/CoNi-LDH composite were investigated as photocatalysts for water remediation,an environmentally motivated ***,the photocatalytic degradation of tetracycline was studied as a model *** performance of the supports and composite catalyst were determined by evaluating both the degradation and adsorption *** influence of several experimental parameters such as catalyst loading,pH,and tetracycline concentrationwere *** current study provides important data for water treatment and similar environmental protection applications.

关键词： Layered double hydroxides(LDHs) g-C_(3)N_(4) Plasmonic Ag NPs Photocatalyst,Tetracycline(TC)

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Towards Improved Steroid Hormone Analysis: The Shift from Immunoassays to Mass Spectrometry

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Journal of Analysis and Testing 2025年第01期 118-135页

作者： Bowen Deng Mengxin Bi Yuanyuan Zheng Dilshad Hussain Sen Yang Di Chen Henan Key Laboratory of Nanomedicine for Targeting Diagnosis and Treatment Zhengzhou University International center for Chemical and Biological Sciences HEJ Research Institute of Chemistry University of Karachi

Steroid hormones, synthesized from cholesterol via cytochrome P450 enzymes, are categorized into adrenocortical hormones and sex hormones. Their monitoring is crucial in clinical and research settings for evaluating disease risk and physiological shifts, as well as for managing medical conditions. The structural similarity and concentration differences of steroid hormones in biological samples create significant challenges for analysis. Traditional immunoassays(IAs) are now less effective due to cross-reactivity and other limitations. Advances in mass spectrometry(MS), especially liquid chromatography-tandem mass spectrometry, have become preferred for steroid hormone detection, establishing a new “gold standard” in the field. The paper examines the influence of various pretreatment methods on the sensitivity and detection limits of steroid hormones,including protein precipitation, liquid–liquid extraction, solid-phase extraction, cold-induced phase separation technique,and derivatization technique, providing a crucial reference for clinical steroid detection. This paper reviews IAs and MS methods used recently(2013–2023) for detecting endogenous steroid hormones, highlighting their analytical strengths and limitations. It also discusses recent advancements and future prospects in both IA and MS methodologies.

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Unilamellar MnO_(2)nanosheets confined Ru-clusters combined with pulse electrocatalysis for biomass electrooxidation in neutral electrolytes

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Science Bulletin 2025年第2期70卷 193-202页

作者： Yuanqing He Chongyang Ma Shiheng Mo Chung-Li Dong Wei Chen Shuo Chen Huan Pang Renzhi Ma Shuangyin Wang Yuqin Zou School of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China State Key Laboratory of Chem/Bio-Sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical EngineeringThe National Supercomputer Centers in ChangshaHunan UniversityChangsha 410082China Department of Physics Tamkang UniversityNew Taipei City 25137China School of Materials Science and Engineering Central South UniversityChangsha 410083China International research center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)TsukubaIbaraki 305-0044Japan

The electrochemical oxidation of 5-hydroxymethylfurfural(HMFOR)in alkaline electrolyte is a promising strategy for producing high-value chemicals from biomass ***,the disproportionation of aldehyde groups under strong alkaline conditions and the polymerization of HMF to form humic substances can impact the purity of 2,5-furandicarboxylic acid(FDCA)*** use of neutral electrolytes offers an alternative environment for electrolysis,but the lack of OH^(-)ions in the electrolyte often leads to low current density and low yields of *** this study,a sandwich-structured catalyst,consisting of Ru clusters confined between unilamellar MnO_(2)nanosheets(S-Ru/MnO_(2)),was used in conjunction with an electrochemical pulse method to realize the electrochemical conversion of5-hydroxymethylfurfural into FDCA in neutral *** electrolysis and the strong electron transfer between Ru clusters and MnO_(2)nanosheets help maintain Ru in a low oxidation state,ensuring high *** increased*OH generation led to a groundbreaking current density of 47 mA/cm^(2)at1.55 V *** hydrogen electrode(RHE)and an outstanding yield rate of 98.7%for FDCA in a neutral *** work provides a strategy that combines electrocatalyst design with an electrolysis technique to achieve remarkable performance in neutral HMFOR.?2024 Science China *** by Elsevier *** Science China *** rights are reserved,including those for text and data mining,AI training,and similar technologies.

关键词： Electrocatalytic 5-hydroxymethylfurfural oxidation Neutral electrolyte Electrocatalysts Nano-confined structure Electrochemical pulse

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