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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 Engineering Institute of Fine Chemicals School of Chemistry and Molecular Engineering East China University of Science and Technology State Key laboratory of Bioreactor Engineering Shanghai Frontier Science Research Base of Optogenetic Techniques for Cell MetabolismEast China University of Science & Technology

Sequence-activated chemiluminescence(CL) technique offers a unique approach to detecting specific biomolecules or cellular events with high sensitivity and spatial resolution. The 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 conditions. This sequential activation could be triggered by enzymes, reactive oxygen species(ROS), biothiols or changes in the microenvironment. These unique sequence-activated CL probes bestow several advantages, including minimal background, deep-tissue penetration, and the ability of non-invasive or minimally invasive detection. The sequence-activated CL techniques represent a significant advancement in molecular imaging and diagnostics. In 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

Visualization of the protective role of estrogen against female liver fibrosis via an ER viscosity NIR fluorescent probe

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Science China Chemistry 2025年第1期68卷 360-368页

作者： Zheng Liu Changyu Zhang Zipeng Li Wanying Ma Jia Liu Xiang Xia Ning Xu Wen Sun Jianjun Du Jiangli Fan Xiaojun Peng State Key laboratory of Fine chemicals Dalian University of Technology Ningbo Institute of Dalian University of Technology

Endoplasmic reticulum(ER) viscosity has emerged as a new potential biomarker for hepatic fibrosis(HF). Herein, we report the first ER-targeting viscosity-responsive near-infrared(NIR) fluorescent probe HBT-PP for investigations of HF *** twisted intramolecular charge transfer(TICT) and the excited state intramolecular proton transfer(ESIPT) are combined to endow HBT-PP with the selective response towards viscosity(～62-fold) and a super large stokes shift(～320 nm). HBT-PP mainly targets organelle ER and is able to image the drug-or alcohol-induced viscosity elevation in living cells. Significantly,HBT-PP was successfully applied to visualize the gender difference in HF and the protective role of estrogen in restraining HF progression. Of note, after 10 min of stain with HBT-PP, HF lesions showed a stage-based response, indicating the potential of this probe in fast and early diagnosis of HF. These results clearly demonstrated the promising application of HBT-PP as a new tool for exploring ER viscosity-involved physiological and pathological processes.

关键词： NIR fluorescent probe ER viscosity hepatic fibrosis gender difference estrogen

Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang State Key laboratory of Fine chemicals School of Chemical Engineering Dalian University of Technology State Key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： Aspect ratio

Electrocatalytic selective synthesis and tandem utilization of hydroxylamine

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Science China Chemistry 2025年

作者： Yuxuan Lu Hengquan Yang Engineering Research Center of Ministry of Education for Fine chemicals School of Chemistry and Chemical Engineering Shanxi Key Laboratory of Green Catalytic Synthesis of Coal-based High Value Chemicals Shanxi University

The transformation of renewable nitrogen feedstock to nitrogenous chemicals plays a significant role in our modern society,considering the crucial impact of nitrogenous chemicals on life sciences,biomedicine,agriculture,and *** （NH2OH）,a typical nucleophile,has been widely served as the nitrogenous feedstock to produce nitrogenous *** NH2OH synthesis methods rely on harsh reaction conditions,leading to an unfavorable environmental *** contrast,nitric oxide electroreduction promises to produce NH2OH powered by renewable *** achievements have revealed the possibility of this process,but have also identified significant *** activity and selectivity are fundamentally limited by competing hydrogenation reactions,while the performance evaluation with high accuracy and reproducibility is ***,this review aims to provide insight into the mechanism of NH2OH electrosynthesis,especially regarding understanding reaction pathways and the design principle towards efficient ***,the performance evaluation parameters and standard measurement methods for NH2OH synthesis are summarized to screen efficient ***,the prospects and emerging opportunities to synthesize nitrogen-containing organic compounds by tandem reaction are *** review aims to provide a guide for evaluating and exploring efficient electrocatalytic systems for NH2OH production and utilization technology.

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Spin-modulated near-infrared-Ⅰ emission in a xanthene-decorated Fe(Ⅱ) spin-crossover complex

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Science China Chemistry 2025年

作者： Cheng Yi Duyong Chen Shihui Zhang Rui Cai Chunying Duan Yinshan Meng Tao Liu State Key laboratory of Fine chemicals Frontier Science Center for Smart Materials and Chemical Engineering School of Chemical Engineering Dalian University of Technology Instrumental Analysis Center Dalian University of Technology School of Chemistry Dalian University of Technology Liaoning Binhai laboratory

Molecular materials showing synergetic coupling of near-infrared （NIR） fluorescence and spin-crossover （SCO） are promisingly applicable in in-vivo bioimaging,temperature sensing,and spintronic *** the related study faces formidable *** this work we graft the NIR fluorophore xanthene onto the dipyridyl substituted triazole ligand and construct a new Febased SCO material,{FeⅡ（ddxc-abpt）2[N（CN）2]2}(1,ddxc-abpt:（E）-4-(((3,5-di（pyridin-2-yl）-4H-1,2,4-triazol-4-yl)imino)methyl)-N,N-diethyl-2,3-dihydro-1H-xanthen-6-amine).Magnetic studies indicate that compound 1 exhibits thermally induced SCO property in both the solid and solution ***-temperature fluorescence emission spectra reveal a remarkable 7-fold increase in photoluminescence intensity upon the transition from the low-spin state at 110 K to the high-spin state at 280 K,which is the record of all reported coupled fluorescence-SCO ***-temperature ultraviolet-visible （UV-Vis）absorption spectra show a significant change in absorption intensity within the fluorescence emission window,consistent with the F?rster resonance energy transfer （FRET） ***-dependent density functional theory （TD-DFT） calculations demonstrate that the strong coupling is attributed to disrupted energy transfer between the xanthene fluorophore and high-spin *** work provides a feasible approach for expanding the synergetic SCO-fluorescence materials to the NIR-Iwavelength region,and hopefully contributes to the applications of tunable NIR-SCO molecule-based sensors and devices.

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Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou State Key laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Advanced Membranes and Porous Materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Institute of Sustainability for chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of Materials Science and Engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Activation energy

Atmospheric reductive catalytic fractionation of lignocellulose integrated with one-pot catalytic conversion of carbohydrate yielding valuable lignin monomers and platform chemicals from corn straw

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Green Energy & Environment 2025年第1期10卷 161-172页

作者： Meng-Ying Liu Zhe-Hui Zhang Xue-Qi Wang Qian Sun Chen Zhang Yu Li Zhuohua Sun Katalin Barta Feng Peng Tong-Qi Yuan State Key laboratory of Efficient Production of Forest Resources Beijing Forestry UniversityBeijing100083China Beijing Key laboratory of Lignocellulosic Chemistry Beijing Forestry UniversityBeijing100083China Department of Chemistry Organic and Bioorganic ChemistryUniversity of GrazHeinrichstrasse 28/II8010 GrazAustria

Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent ***,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps *** key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene *** utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling *** the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.

关键词： Atmospheric reductive catalytic fractionation Corn straw Ethylene glycol Raney Ni 5-Methoxymethylfurfural

Tailor-made high elasticity and low-hysteresis hydrogels based on asymmetric H-bonding crosslinking for wearable applications

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Science China Chemistry 2025年

作者： Xiaofang Shi Nan Shi Miaomiao Dang Chengyu Ji Yingjie Li Peiyi Wu Zhiguo Hu Collaborative Innovation Centre of Henan Province for Green Manufacturing of Fine chemicals Henan Engineering Laboratory of Chemical Pharmaceutical and Biomedical Materials School of Chemistry and Chemical Engineering Henan Normal University State Key laboratory for Modification of Chemical Fibers and Polymer Materials College of Chemistry Chemical Engineering and Biotechnology & Center for Advanced Low-dimension Materials Donghua University

The conventional method of fabricating hydrogels constantly confronts the conflict between elasticity and toughness, limiting their repetitive application. Achieving the desired elasticity through a simple and low-cost approach is a significant challenge for hydrogels, particularly through rational molecular design. Here, low-hysteresis and high-toughness hydrogels are developed from the design of a new feature monomer, N-acryloylethylsemicarbazide (NACE). Based on a concept of “asymmetric Hbonding design”, the unique double and triple H-bonding of NACE can result in a novel asymmetric crosslinking polymer with alternating strong and weak H-bonding regions. The NACE is copolymerized with acrylamide (AM) to regulate the mechanical properties of hydrogel via H-bonding density. The P(NACE-AM) ionic hydrogels are obtained simply and rapidly via one-step photopolymerization without a chemical cross-linking agent. The P(NACE-AM) hydrogels combine superb mechanical elasticity and toughness, and excellent ionic conductivity, showing great potential as durable ionic conductive devices for wearable utilization.

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CO2-mediated bicarbonate conversion to concentrated formate in a CEM-based electrolyzer

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Journal of Energy Chemistry 2025年第1期100卷 605-611页

作者： Haocheng Xiong Donghuan Wu Haonan Li Andrew Li Qikun Hu Siyao Song Bingjun Xu Qi Lu State Key laboratory of Chemical Engineering Department of Chemical Engineering Tsinghua University College of Chemistry and Molecular Engineering Peking University Ordos laboratory

Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO2emissions,as bicarbonate can be efficiently generated from the capture of atmospheric CO2using alkaline solutions with reactive *** this work,we present a CO2-mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm2electrode *** electrolysis achieved selectivities exceeding 75%for formate at a total current of 2.5 A,achieving formate concentrations up to 1.2 M and yields as high as 95%over extended *** techno-economic assessment confirmed the economic viability of the process,highlighting the potential for bicarbonate electrolysis as a sustainable method for producing valuable chemicals.

关键词： Electrocatalysis Techno-economic assessments Electrochemistry Flow electrolyzer

A light-regulated synthetic ion channel constructed by an azobenzene modified hydraphile

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Chinese Chemical Letters 2015年第7期26卷 851-856,920页

作者： Rong-Yan Yang Chun-Yan Bao Qiu-Ning Lin Lin-Yong Zhu Shanghai Key laboratory for functional Materials Chemistry Institute of Fine Chemicals East China University of Science and Technology

Biological ion channels are key molecules for cellular regulation and communication. To mimic the structure and functions of nature ion channels, a new class of light-regulated transmembrane ion channels was reported based on tri（macrocycle） hydraphile and azobenzene photoswitch （hydraphile 1 ）. The liposome-based proton transport assays showed that hydraphile 1 exhibited excellent transmem- brane activity （Y）, and Ymax arrived 0.7 at 40 μmol/L. The successful isomerization of azohenzene moiety was confirmed and qualified by UV and NMR spectra. Upon alternative irradiation of 365 nm UV light and 450 nm visible light, the transmembrane activity of hydraphile I was regulated between 0.35 and 0.5, reversibly. All the obtained results have demonstrated the promise of developing excellent synthetic ion channels with ion gating properties based on simple molecular design.

关键词： Synthetic ion channelLight-regulated ion transportHydraphilesAzobenzene photoisomerizationSelf-assembly

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