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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao Yifu Yu Department of chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

Ordered Bicontinuous Network Structures Regulated by Orientational Interactions in a Rod-Coil Block Copolymer

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Chinese Journal of Polymer science 2024年第5期42卷 636-642,I0008页

作者： Xiao-Lin Lyu Shi-Chu Yang An-Qi Xiao Ping-Ping Hou Wei Zhang Hong-Bing Pan Zhi-Hao Shen Xing-He Fan Qi-Feng Zhou Beijing National Laboratory for molecular sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Key Laboratory of Advanced Materials Technologies International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials TechnologiesCollege of Materials Science and EngineeringFuzhou UniversityFuzhou350108China

The rich phase behavior of block copolymers(BCPs)has drawn great attention in recent ***,the double diamond(DD)phase is rarely obtained because of the competition between the minimization of interfacial energy and packing ***,a rod-coil BCP containing mesogen-jacketed liquid crystalline polymer is designed to acquire ordered bicontinuous network *** reduction of internal energy originating from the orientational interaction among the rod blocks can compensate for the free energy penalty of packing frustration to stabilize the DD *** resulting BCP can also experience lamellae-to-DD and double gyroid-to-lamellae transitions by changing the annealing *** results make the rod-coil BCP an excellent candidate for the self-assembly of ordered network structures,demonstrating great potential in nanopatterning and metamaterials.

关键词： Block copolymer Rod-coil Ordered bicontinuous phase Double diamond Double gyroid

MoO_(x) nanoclusters on Mo-doped TiO_(2) nanosheets with enhanced singlet oxygen generation and sulfide conversion abilities for photocatalytic aerobic oxidative desulfurization

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science China chemistry 2024年第1期67卷 408-414页

作者： Suting Xie Xinyu Zhao Dongxiao Wang Huawei Yang Lixia Yang Liangjiu Bai Donglei Wei Wenxiang Wang Ying Liang Hou Chen Shaojun Guo college of chemistry and Materials science Ludong UniversityYantai 264025China college of Materials science and Engineering Peking UniversityBeijing 100871China

Photocatalytic aerobic oxidation desulfurization(PAODS)is a promising and sustainable alternative to conventional,energyintensive desulfurization techniques for petroleum ***,its development is greatly plagued by the low capability in generating highly reactive oxygen species and sluggish kinetics of sulfide oxidation of reported *** we report a class of MoO_(x)nanocluster decorated on ultrathin Mo-doped TiO_(2)nanosheet(MoO_(x)/MoTiO)catalyst for efficiently facilitating the photocatalytic aerobic oxidation of *** demonstrate that MoO_(x)/MoTiO can not only promote the generation of highly reactive singlet oxygen(^(1)O_(2))but also enhance the aerobic conversion of sulfides,which leads to a record dibenzothiophene oxidation activity of 3.90 mmol g^(-1)h^(-1).The multiple experimental characterizations and density functional theory calculations collectively reveal that the doped-Mo sites can interact with the photogenerated excitons,enabling directly energy transfer generation of^(1)O_(2)through a new exciton modulation mechanism,and the coordination unsaturated MoO_(x)clusters play the role of co-catalyst to enhance the separation of charge carriers,and effectively catalyze the reaction between sulfides and1O_(2)to form sulfones.

关键词： titanium dioxide photocatalytic aerobic oxidation desulfurization dibenzothiophene singlet oxygen

Atomic Ni directional-substitution on ZnIn_(2)S_(4) nanosheet to achieve the equilibrium of elevated redox capacity and efficient carrier-kinetics performance in photocatalysis

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Journal of Energy chemistry 2024年第1期88卷 272-281,I0007页

作者： Haibin Huang Guiyang Yu Xingze Zhao Boce Cui Jinshi Yu Chenyang Zhao Heyuan Liu Xiyou Li School of Materials science and Engineering China University of Petroleum(East China)Qingdao 266580ShandongChina Key Laboratory of Optic-electric Sensing and Analytical chemistry for Life science(MOE) College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina college of New Energy China University of Petroleum(East China)Qingdao 266580ShandongChina

It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic ***,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal *** electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction *** the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface ***,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.

关键词： ZnIn_(2)S_(4) Substitution Carrier kinetics Redox capacity Photocatalysis

Colorimetric and Photothermal Dual-modal Visual Detection of Iodide Ion Based on G-Quadruplex-Hemin Cascade Signal Amplification

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Chemical Research in Chinese Universities 2024年第2期40卷 305-310页

作者： CHEN Yanyue LIU Jiali LIU Jiawen HU Rong YANG Yunhui ZHANG Xiaobing college of chemistry and Chemical Engineering Yunnan Normal UniversityKunming650500P.R.China molecular science and Biomedicine Laboratory State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringCollaborative Innovation Center for Molecular Engineering for TheronasticsHunan UniversityChangsha410082P.R.China

The insufficient internal resorption of iodide ions(I−)leads to thyroid disorders,such as goiter,hypothyroidism,and cretinism in *** this paper,a portable point-of-care testing(POCT)platform was developed for the dual-modal analysis of I^(−),seamlessly integrating both colorimetric and photothermal thermometer *** quantification of results was achieved using a standard thermometer or smartphone.G-Quadruplex/Hemin(G4/Hemin)is the DNAzyme with peroxidase-like *** catalytic efficacy of G-quadruplex structures can be enhanced with the help of I^(−),manifesting as multicolor transitions from colorless to green and then blue,and accompanied by the increase of temperature,which can be used for the quantitative detection of I^(−).Additionally,digital analysis according to the three-color channels(R/G/B)by a cellphone eliminated the requirement for intricate *** dual-modal method for portable I^(−)determination is cost-effectiveness,simplicity,remarkable sensitivity(0.5 nmol/L)and ***,it was applied to determining the concentration of I^(−)in spiked serum samples.

关键词： Dual-modal platform G-Quadruplex Iodide ion Point-of-care testing(POCT) Aptasensor

Amplifiable protein identification via residue-resolved barcoding and composition code counting

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National science Review 2024年第7期11卷 205-217页

作者： Weiming Guo Yuan Liu Yu Han Huan Tang Xinyuan Fan Chu Wang Peng R.Chen Synthetic and Functional Biomolecules Center Beijing National Laboratory for Molecular SciencesKey Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University Peking-Tsinghua Center for Life sciences Academy for Advanced Interdisciplinary Studies Peking University

Ultrasensitive protein identification is of paramount importance in basic research and clinical diagnostics but remains extremely challenging. A key bottleneck in preventing single-molecule protein sequencing is that, unlike the revolutionary nucleic acid sequencing methods that rely on the polymerase chain reaction(PCR) to amplify DNA and RNA molecules, protein molecules cannot be directly amplified. Decoding the proteins via amplification of certain fingerprints rather than the intact protein sequence thus represents an appealing alternative choice to address this formidable challenge. Herein, we report a proof-of-concept method that relies on residue-resolved DNA barcoding and composition code counting for amplifiable protein fingerprinting(AmproCode). In AmproCode, selective types of residues on peptides or proteins are chemically labeled with a DNA barcode, which can be amplified and quantified via quantitative PCR. The operation generates a relative ratio as the residue-resolved ‘composition code’ for each target protein that can be utilized as the fingerprint to determine its identity from the proteome database. We developed a database searching algorithm and applied it to assess the coverage of the whole proteome and secretome via computational simulations, proving the theoretical feasibility of AmproCode. We then designed the residue-specific DNA barcoding and amplification workflow, and identified different synthetic model peptides found in the secretome at as low as the fmol/L level for demonstration. These results build the foundation for an unprecedented amplifiable protein fingerprinting method. We believe that, in the future,AmproCode could ultimately realize single-molecule amplifiable identification of trace complex samples without further purification, and it may open a new avenue in the development of next-generation protein sequencing techniques.

关键词： protein identification amplifiable fingerprinting residue-specific chemistry DNA barcoding composition code counting

Universal synthesis of metallophthalocyanine covalent organic frameworks as ultra-sensitive multifaceted electrochemical sensor

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science China chemistry 2024年第6期67卷 2092-2101页

作者： Qi Liu Qiqi Sun Yuming Zhang Hao Li Wenmiao Chen Yuexing Zhang Sirong Yu Yanli Chen Jianzhuang Jiang School of Materials science and Engineering China University of Petroleum(East China)Qingdao266580China Beijing Key Laboratory for science and Application of Functional molecular and Crystalline Materials School of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing100083China college of chemistry and Chemical Engineering Dezhou UniversityDezhou253023China

The universal synthesis of highly stable covalent organic frameworks(COFs)for ultra-sensitive and multi-component electrochemical detection in different scenarios remains a great ***,a series of metallophthalocyanine-based twodimensional(2D)dioxin(DXI)-linked metalophthalocyanine(MPc)-n DXI-COFs(M=Ni,Zn;n=1,2)are afforded in high yield(80%-96%)by a facile trace-quinoline assisted one-pot condensation of tetracarbonitrile *** X-ray diffraction and electron microscopy investigations disclose their lamellar texture 2D network with AA stacking *** and calculation results elucidate that the 2DXI-linked MPc-2DXI-COFs provide the stronger built-in electronic field and more electrostatic/hydrogen bonding adsorption sites than DXI-linked MPc-DXI-COFs,and the lower electrode reaction Gibbs free energy and stronger adsorption of analytes at Ni Pc than Zn Pc unit,which grants Ni Pc-2DXI-COF excellent sensing properties for various analytes including neurotransmitters,organic pollutants,and heavy metal ions,with high sensitivity and low detection limit of 0.53 to 25.66 *** in binary and ternary systems and even in real-world conditions,simultaneous multi-component detection could be achieved.

关键词： covalent organic framework metallophthalocyanine 2D materials electrochemical sensors multi-component detection

Crystalline-amorphous M@MN_x(M=Co,Fe,Ni)encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： Yang Yang Xiao-Chuan Duan Shao-Hui Guo Xian-Ming Zhang college of Materials science and Engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of TechnologyYuci030600China

Developing earth-abundant electrocatalysts for hydrogen evolution reaction(HER)is important for the sustainable energy ***,efficient and stable heterocatalysts consisting of crystalline-amorphous M@MN_(x)(M=Co,Fe,Ni)encapsulated in N-doped carbon layers supported with N-doped graphene sheets(denoted as M@MN_(x)@NC-NG)are synthesized by facile hydrothermal reaction and nitridation *** the nitriding process,metal ions in M(tzbc)_2(H_(2)O)_4(tzbc=4-(1H-1,2,4-triazol-1-yl)benzoic acid)complexes are reduced to crystalline M cores,accompanied by the formation of amorphous MN_(x)shells;the tzbc ligands are insitu carbonized to form outermost N-doped carbon(NC)layers that connect with inner MN_(x)via M-N-C motifs inherited from the complex precursors and inhibit the transition of MN_(x)from amorphous to crystalline *** Co@CoN_(x)@NC-NG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm^(-2)and low Tafel slopes of 40 and 85 mV·dec^(-1)in 0.5 mol·L^(-1)H_(2)SO_4 and1.0 mol·L^(-1)KOH electrolytes,*** Co@CoN_(x)@NC-NG retains 97%of the initial overpotential after 100,000 s in both acidic and alkaline *** outstanding HER performance originates from the crystalline-amorphous Co@CoN_(x)that redistributes electrons around the heterointerfaces,facilitating the conversion process of H^(+)/H_(2)O to hydrogen and thereby promoting HER *** outermost NC layers serve as the armor of Co@CoN_(x),and graphene nanosheets act as carriers of egg-like Co@CoN_(x)@NC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

Nanomaterial Assisted Exosome Analysis Using Mass Spectrometry

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Chemical Research in Chinese Universities 2024年第2期40卷 237-254页

作者： ZHANG Yi ZHOU Bokai LI Qiuning JIN Mingshi BAI Yu Beijing National Laboratory for molecular sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871P.R.China Department of chemistry Yanbian UniversityYanji133002P.R.China

Exosomes,extracellular vesicles(EVs)that play crucial roles in biological processes,have emerged as attractive targets for noninvasive disease diagnosis and *** spectrometry(MS)offers high sensitivity,high throughput,and excellent qualification and quantification capacity,which is the ideal approach for exosome ***’unique physiochemical properties,controllable morphology,and large surface area make them promising in biological sample pretreatment and *** contributed diverse functions to the exosome MS analysis,encompassing substrates for exosome isolation and cargos enrichment,matrices for laser desorption/ionization(LDI),read-out signals and supporters for signal amplification strategies,*** this review,recent progress in the applications of nanomaterial in the exosome MS analysis was summarized and a comprehensive discussion on the challenges and perspectives was proposed for the development of an advancing analysis approach of exosomes for the accurate diagnosis and monitoring of diseases.

关键词： Exosome Nanomaterial Enrichment Matrix Mass spectrometry

RuO_(2)/TiO_(2)/MXene with multi-heterojunctions coating on carbon cloth for high-activity chlorine evolution reaction at large current densities

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Nano Research 2024年第6期17卷 4764-4772页

作者： Yuhao Duan Liuxu Wei Chenyu Cai Junbao Mi Fuyuan Cao Jiaze Chen Xiaolong Li Xiujiang Pang Bin Li Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationInternational Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China college of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042China college of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China

The chlorine evolution reaction(CER)is a crucial step in the production of chlorine gas and active chlorine by chlor-alkali ***,the endeavor to fabricate electrodes capable of yielding high current density at minimal overpotential remains a central challenge in advancing the realm of chlorine evolution ***,we grow TiO_(2)and RuO_(2)on MXene@carbon cloth(CC)through the favorable affinity and induced deposition effect between the surface functional groups of MXene and the metal.A self-supported electrode(RuTiO_(2)/MXene@CC)with strong binding at the electrocatalyst-support interface and weak adhesion at electrocatalyst-bubble interface is *** RuTiO_(2)/MXene@CC can reduce the electron density of RuO_(2)by regulating the electron redistribution at the heterogeneous interface,thus enhancing the adsorption of Cl−.RuTiO_(2)/MXene@CC could achieve a high current density of 1000 mA·cm^(−2)at a small overpotential of 220 mV,superior to commercial dimensionally stable anodes(DSA).This study provides a new strategy for constructing efficient CER catalysts at high current density.

关键词： chlorine evolution reaction high current density MXene TiO_(2) RuO_(2)