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Revealing the difference of Stark tuning rate between interface and bulk by surface-enhanced infrared absorption spectroscopy

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Chinese Chemical Letters 2025年第2期36卷 461-464页

作者： Manyu Zhu Fei Liang Lie Wu Zihao Li Chen Wang Shule Liu Xiue Jiang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences School of applied chemistry and engineering University of Science and Technology of China School of Materials Science and engineering Sun Yat-sen University Research Center for Analytical Science College of ChemistryNankai University

Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric *** using surface-enhanced infrared absorption(SEIRA) spectroscopy,attenuated total reflection (ATR) spectroscopy and molecular dynamics (MD),we reveal the assembled C≡N at gold nanofilm exhibits a reduced Stark tuning rate (STR) referring to the vibrational frequency shift in response to electric field comparing with the bulk which was regulated by the electron transfer between S and *** findings lead to a deeper understanding of the vibrational Stark effect at the interface and provide guidance for improving the interface electric field theory.

关键词： Attenuated total reflection spectroscopy Cyano group Stark tuning rate Surface-enhanced infrared spectroscopy Vibrational stark effect

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

Investigation on Cu promotion effect on Ce-based solid solution-anchored Rh single atoms for three-way catalysis

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Chinese Chemical Letters 2025年第2期36卷 574-578页

作者： Jianing He Xiao Wang Zijian Wang Ruize Jiang Ke Wang Rui Zhang Huilin Wang Baokang Geng Hongyi Gao Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of applied chemistry and engineering University of Science and Technology of China China School of Materials Science and engineering University of Science and Technology Beijing Department of chemistry Tsinghua University

The three-way catalyst（TWC）, as a promising approach to control automobile exhaust emission, has been widely studied and applied. However, it still suffers from the high light-off temperature and poor ***, we synthesized a multicomponent catalyst Rh/Cu-CeSn by using Cu metal doping to modify the Ce-based solid solution, which exhibited good TWC catalytic performance: the light-off temperatures for CO, NO, and C3H6conversion are 172 ℃, 266 ℃, and 193 ℃, respectively. Moreover, the catalyst still maintained good activity after 12 h of the continuous reaction under high-temperature conditions. The experiments and mechanism studies reveal that due to the redox pair Cu+/Cu2+, the Cu incorporation can effectively inhibit the Rh transition to the oxidation state and greatly enhance the catalytic activity and stability. This work provides a viable strategy for precise characteristic modulation of composite oxide supports during the fabrication of noble metal-based catalysts, which significantly reduces environmental pollution from energy applications.

关键词： Co-precipitation Oxygen vacancies Rhodium (Rh) catalyst Solid solution Three-way catalysts (TWC)

De novo synthesis of atropisomeric benzofurans via Cu/SPDO complex catalyzed asymmetric formal[3+2]annulation

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Science China chemistry 2025年第1期68卷 174-180页

作者： Fan-Xiao Meng Xing-Yu Wang Ka Lu Ju-Song Yang Fu-Min Zhang Ai-Jun Ma Bao Du Yong-Qiang Tu State Key Laboratory of applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China School of chemistry and Chemical engineering Shanghai Jiao Tong UniversityShanghai 200240China School of Biotechnology and Health Sciences Wuyi UniversityJiangmen 529020China

Herein,the de novo synthesis of atropisomeric benzofurans through the Cu/spirocyclic-pyrrolidine-oxazoline(SPDO)complex catalyze asymmetric formal[3+2]cycloaddition between quinones and ynamides is explored,producing a range of structurally diverse axially chiral benzofurans in satisfactory yields with good to excellent ***,density functional theory calculations were applied to explain the possible reaction mechanism.

关键词： benzofuran atropisomers novel de novo synthetic strategy asymmetric formal[3+2]cycladdition Cu/SPDO complex DFT calculations

A Computer Simulation Study on Deposition Patterns of Cyclic Diblock Copolymer Solution Nanodroplets:Influence of Polymer Length and Concentration

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Chemical Research in Chinese Universities 2025年第1期41卷 21-32页

作者： PEI Hanwen ZHANG Jun SUN Zhaoyan State Key Laboratory of Polymer Physics and chemistry&Key Laboratory of Polymer Science and Technology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022P.R.China School of applied chemistry and engineering University of Science and Technology of ChinaHefei230026P.R.China

Molecular dynamics simulations are conducted to investigate the deposition patterns of cyclic diblock copolymer solution nanodroplets on solid surfaces(walls).The primary focus is how initial polymer concentration,chain length,and solvent-wall interaction affect these *** patterns are categorized into phase diagrams,mainly composed of multihollow,coffee-ring,and multilayer *** also study the deposition of polymer blocks with different adsorption behavior by adjusting the interaction strength between the polymer block and the wall[ε_(A(B)W)],including weakly adsorbable(ε_(A(B)W)=0.6),moderately adsorbable(ε_(A(B)W)=1.0),and strongly adsorbable(εA(B)W=1.2)polymer *** study identifies the key factors influencing the droplet’s deposition structure and elucidates the mechanisms behind pattern *** findings contribute to the design of deposition patterns for cyclic diblock copolymer solution nanodroplets,enhancing applications related to droplet evaporation.

关键词： Cyclic diblock copolymer Nanodroplet Evaporation Deposition pattern Chain length and concentration

The study of antibacterial activity of cationic poly(β-amino ester)regulating by amphiphilic balance

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Chinese Chemical Letters 2025年第2期36卷 332-336页

作者： Chong Liu Ling Li Jiahui Gao Yanwei Li Nazhen Zhang Jing Zang Cong Liu Zhaopei Guo Yanhui Li Huayu Tian School of Materials Science and engineering Changchun University of Science and Technology School of Materials Science and engineering Xiamen University of Technology Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied Chemistry Chinese Academy of Sciences College of chemistry and Chemical engineering Xiamen University

It is well known that cationic polymers have excellent antimicrobial capacity accompanied with high biotoxicity, to reduce biotoxicity needs to decrease the number of cationic groups on polymers, which will influence antimicrobial activity. It is necessary to design a cationic polymer mimic natural antimicrobial peptide with excellent antibacterial activity and low toxicity to solve the above dilemma. Here,we designed and prepared a series of cationic poly(β-amino ester)s(PBAEs) with different cationic contents, and introducing hydrophobic alkyl chain to adjust the balance between antimicrobial activity and biotoxicity to obtain an ideal antimicrobial polymer. The optimum one of synthesized PBAE(hydrophilic cationic monomer:hydrophobic monomer = 5:5) was screened by testing cytotoxicity and minimum inhibitory concentration(MIC), which can effectively kill S. aureus and E. coli with PBAE concentration of15 μg/m L by a spread plate bacteriostatic method and dead and alive staining test. The way of PBAE killing bacterial was destroying the membrane like natural antimicrobial peptide observed by scanning electron microscopy(SEM). In addition, PBAE did not exhibit hemolysis and cytotoxicity. In particular, from the result of animal tests, the PBAE was able to promote healing of infected wounds from removing mature S. aureus and E. coli on the surface of infected wound. As a result, our work offers a viable approach for designing antimicrobial materials, highlighting the significant potential of PBAE polymers in the field of biomedical materials.

关键词： Amphiphilic balance Antimicrobial Cationic polymers Michael addition polymerization Poly(β-amino ester)s

Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO_(2)reduction to C2þchemicals

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Green Energy & Environment 2025年第2期10卷 422-432页

作者： Wenrui Wan Fanhua Meng Si Chen Jianhua Wang Chunyan Liu Yan Wei Chenpu He Li Fan Qiaolan Zhang Weichun Ye Huanwang Jing State Key Laboratory of applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000GansuChina Key Laboratory of Green Chemical Media and Reactions(Ministry of Education) School of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang453007HenanChina School of Chemical engineering Lanzhou University of Arts and SciencesLanzhou730010China

Converting CO_(2)and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy *** inspiration from the structures of natural leaves,we designed and synthesized a novel copper-coordinated covalent triazine framework(CuCTF)supported by silicon nanowire arrays on wafer *** marks the first-ever application of such a hybrid material in the photoelectrocatalytic reduction of CO_(2)under mild *** Si@CuCTF6 heterojunction has exhibited exceptional selectivity of 95.6%towards multicarbon products(C^(2+))and apparent quantum efficiency(AQE)of 0.89%for carbon-based *** active sites of the catalysts are derived from the nitrogen atoms of unique triazine ring structure in the ordered porous framework and the abundant Cu-N coordination sites with bipyridine ***,through DFT calculations and operando FTIR spectra analysis,we proposed a comprehensive mechanism for the photoelectrocatalytic CO_(2)reduction,confirming the existence of key intermediate species such as*CO_(2)-,*=C=O,*CHO and*CO-CHO *** work not only provides a new way to mimic photosynthesis of plant leaves but also gives a new opportunity to enter this research field in the future.

关键词： Silicon Photoelectrocatalysis CO_(2)reduction Covalent triazine framework Sustainable chemistry

Transforming waste particles into valuable adsorbents via amyloid-mediated molecular engineering

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Science China chemistry 2025年第1期68卷 317-328页

作者： Qingmin Yang Jian Zhao Yujia Zhang Xingyu Zhou Hao Ren Bowen Hu Zhongli Lei Lixin Chen Peng Yang Key Laboratory of applied Surface and Colloid chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China School of Material and Chemical engineering Bengbu UniversityBengbu 233030China Anhui Provincial engineering Laboratory of Silicon-Based Materials Bengbu 233030China Xi’an Key Laboratory of Polymeric Soft Matter School of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China International Joint Research Center on Functional Fiber and Soft Smart Textile School of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China School of chemistry and Chemical engineering Northwestern Polytechnical UniversityXi’an 710129China

The high-value utilization of industrial solid waste using a facile and eco-friendly process is of great interest and significance in reducing environmental pollution and developing a green circular ***,we propose an amyloid-mediated molecular engineering strategy to transform particulate waste into valuable adsorbents for metal *** method has the advantage of aqueous solution fabrication under mild conditions without the use of high-temperature hydrothermal methods and toxic chemical ***-mediated molecular engineering manipulates the phase transition of bovine serum albumin(BSA)on particulate waste surfaces,resulting in a remarkable~3.1 times improvement in the adsorption capacity of fly ash,a typical industrial solid waste for gold ions after modification with the phase-transitioned BSA(PTB).The resultant adsorption ability was 69–1,980 times higher than those of conventional and emerging adsorbent materials such as ion exchange resins,activated carbon(AC),covalent organic frameworks(COFs),and metal-organic frameworks(MOFs).We further demonstrated the application of our PTB-modified materials in the recovery of precious metals from low-grade gold ore and electronic waste ***,this strategy could increase the value of waste materials nearly 27 *** addition,this method is generally extendable to other conventional industrial adsorbents such as resin,clay,and Al_(2)O_(3),and enhances their adsorption capabilities at least ***,this work provides a simple and green approach for improving the adsorption performance of solid particles,and is expected to develop into a universal strategy for transforming waste particles into high-value-added products.

关键词： amyloid-like protein aggregates surface engineering fly ash solid waste adsorption

Co-loading Pd and CeO_(2)on Silicalite-1 as High-performance Catalyst for Methane Dry Reforming Reaction

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Chemical Research in Chinese Universities 2025年第1期41卷 15-20页

作者： XU Jing ZHANG Rui WANG Ke WANG Xiao SONG Shuyan ZHANG Hongjie State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022P.R.China School of applied chemistry and engineering University of Science and Technology of ChinaHefei230026P.R.China Department of chemistry Tsinghua UniversityBeijing100084P.R.China

The methane dry reforming(DRM)reaction can convert CO_(2)and CH_(4),both of which contribute to climate change,into syngas,which holds great significance in mitigating specific environmental issues stemming from the greenhouse ***,the challenges that persist include the substantial energy consumption and the catalyst’s susceptibility to deactivation,both of which necessitate ***,we developed a catalyst,PdCe/S1,featuring small-sized Pd species and CeO_(2)stabilized on pure silicon zeolite(silicalite-1),which is employed in the DRM *** can achieve 97%CH_(4)conversion and 98%CO_(2)conversion at 750℃,surpassing binary Pd/CeO_(2)and Pd/S1 *** small size of CeO_(2)stabilized by silicalite-1 promotes oxygen defects formation and enhances the CO_(2)adsorption *** introduction of silicalite-1 further enhances the interaction between Pd and CeO_(2),boosting DRM performance.

关键词： Dry reforming of methane CeO_(2) Zeolite