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Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel

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Journal of Energy chemistry 2025年第1期100卷 628-636页

作者： Yi Qi Xueying Chen Bowen Liu Xuliang Lin Xueqing Qiu Yanlin Qin Guangdong provincial key laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Guangdong provincial laboratory of chemistry and fine Chemical Engineering Jieyang Center Guangdong Basic Research Center of Excellence for Ecological Security and Green Development Guangdong University of Technology

Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great *** demonstrate the targeted synthesis and cation modulation of NiCo2O4spinel nanoboxes,synthesized via cation exchange and calcination *** catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and *** catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as *** porous architecture and polymetallic composition of the NiCo2O4spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for *** innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT *** work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.

关键词： Spinel Biomass valorization Electrocatalysis Lignin oxidation Coupling

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A Mn-porphyrinic metal–organic framework immobilizing glucose oxidase for combined photodynamic/chemodynamic/starvation therapy

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Tungsten 2025年第1期7卷 183-194页

作者： Xin-Ran Sun Hao-Ming Yuan Guo-Da Zhang Chao Wang Shu-Juan Sun Peng-Fei Shi Shandong provincial key laboratory of Detection Technology for Tumor Markers School of Chemistry and Chemical Engineering Linyi University

The combination of photodynamic therapy（PDT） and chemodynamic therapy（CDT） in tumor treatment has attracted considerable ***,tumor hypoxia and glutathione（GSH） overproduction in the tumor tissue restricted the progress of their ***,a Mn-porphyrinic metal-organic framework（Mn-TCPP） was constructed by the one-pot method and further used for immobilizing glucose oxidase（GOx） to obtain GOx@*** would rapidly exhaust endogenous glucose into hydrogen peroxide（H2O2） and gluconic acid,thus shutting off the energy supply of tumor cells for starvation ***-TCPP catalyzed H2O2to produce oxygen,regulating the hypoxic tumor microenvironment and in turn improving1O2generation under laser ***,Mn-TCPP can reduce reactive oxygen species consumption owing to the redox reaction between Mn3+and GSH,thus greatly enhancing ***,benefiting from GOx-mediated starvation therapy,Mn2+produced by Mn3+reduction can react with sufficient intracellular H2O2to generate ·OH with high cytotoxicity through a Fenton-like *** treatment by GOx@Mn-TCPP under laser irradiation in vitro,the cell viability of 4T1 and A549 tumor cells reached to 20%,reflecting GOx@Mn-TCPP could give full play to the advantages of PDT/CDT/starvation *** results in vivo demonstrated that GOx@Mn-TCPP mediated synergistic cascade therapy could significantly inhibit tumor growth and improve the therapeutic effect.

关键词： Chemodynamic therapy Immobilizing enzyme Metal–organic frameworks Photodynamic therapy Starvation therapy

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Research progress of catalysts for direct coal liquefaction

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Journal of Energy chemistry 2025年第1期100卷 481-497页

作者： Wei Song Penggao Liu Xinyue Chen Ting Wang Chunrong He Rui Hao Kaiyu Liu State key laboratory of chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University College of chemistry and Chemical Engineering Henan Polytechnic University Hunan provincial key laboratory of Chemical Power Sources College of Chemistry and Chemical Engineering Central South University

Coal direct liquefaction technology is a crucial contemporary coal chemical technology for efficient and clean use of coal resources. The development of direct coal liquefaction technology and the promotion of alternative energy sources are important measures to guarantee energy security and economic security. However, several challenges need to be addressed, including low conversion rate, inadequate oil yield, significant coking, demanding reaction conditions, and high energy consumption. Extensive research has been conducted on these issues, but further exploration is required in certain aspects such as pyrolysis of macromolecules during the liquefaction process, hydrogen activation, catalysts' performance and stability, solvent hydrogenation, as well as interactions between free radicals to understand their mechanisms better. This paper presents a comprehensive analysis of the design strategy for efficient catalysts in coal liquefaction, encompassing the mechanism of coal liquefaction, catalyst construction,and enhancement of catalytic conversion efficiency. It serves as a comprehensive guide for further research endeavors. Firstly, it systematically summarizes the conversion mechanism of direct coal liquefaction, provides detailed descriptions of various catalyst design strategies, and especially outlines the catalytic mechanism. Furthermore, it addresses the challenges and prospects associated with constructing efficient catalysts for direct coal liquefaction based on an understanding of their action mechanisms.

关键词： Direct coal liquefaction Catalysts Mechanism of action Solvent hydrogenation

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Plasmonic tandem heterojunctions enable high-efficiency charge transfer for broad spectrum photocatalytic hydrogen production

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Journal of Energy chemistry 2025年第1期100卷 710-720页

作者： Wenxuan Chen Xiu-Qing Qiao Guo Hui Bojing Sun Dongfang Hou Meidi Wang Xueqian Wu Tao Wu Dong-Sheng Li College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University Hubei Three Gorges laboratory College of chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University

Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer ***,a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo2C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction,Schottky junction,and photothermal *** difference in atomic configuration between cubic-CdS （c-CdS） and hexagonal-CdS （h-CdS） leads to effective charge separation through a typical Ⅱ charge transfer mechanism,and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge ***,the photothermal effect of Mo2C@C helps to expand the light absorption,accelerate charge transfer kinetics,and reduce the hydrogen evolution energy *** carbon layer provides a fast channel for charge transfer and protects the photocatalyst from *** a result,the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H2production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%,surpassing most of the reported *** study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.

关键词： Cadmium sulfide

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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 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

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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

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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 School of Material and Chemical Engineering Bengbu University Anhui provincial Engineering laboratory of Silicon-Based Materials School of chemistry and Chemical Engineering Northwestern Polytechnical University key laboratory of Applied Surface and Colloid chemistry Ministry of Education School of Chemistry and Chemical EngineeringShaanxi Normal University Xi'an key laboratory of Polymeric Soft Matter School of Chemistry and Chemical Engineering Shaanxi Normal University International Joint Research Center on Functional Fiber and Soft Smart Textile School of Chemistry and Chemical EngineeringShaanxi Normal University

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 economy. Herein, we propose an amyloid-mediated molecular engineering strategy to transform particulate waste into valuable adsorbents for metal ions. Our method has the advantage of aqueous solution fabrication under mild conditions without the use of high-temperature hydrothermal methods and toxic chemical reagents. Amyloid-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 leachates. Consequently, this strategy could increase the value of waste materials nearly 27 times. In addition, this method is generally extendable to other conventional industrial adsorbents such as resin, clay, and Al2O3, and enhances their adsorption capabilities at least twofold. Overall, 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

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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

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Engineering atomic Rb-N configurations to tune radical pathways for highly selective photocatalytic H2O2 synthesis coupled with biomass valorization

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Journal of Energy chemistry 2025年第1期100卷 215-225页

作者： Jiaye Li Shuang Pan Yihuang Chen Qiong Liu College of chemistry and Materials Engineering Wenzhou University Guangdong provincial key laboratory of Chemical Measurement and Emergency Test Technology (China) Institute of Analysis Guangdong Academy of Sciences (China National Analytical CenterGuangzhou)

Photocatalytic oxygen reduction for hydrogen peroxide （H2O2） synthesis presents a green and costeffective production ***,achieving highly selective H2O2synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative ***,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H2O2and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride（CNRb）.The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h-1for H2O2generation and photooxidation rate of 3.75 mM h-1for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion （SCC） efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical *** is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product *** study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H2O2coupled with biomass valorization.

关键词： Free radical reactions

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Strategies for achieving fast-charge and high-voltage polymer-based solid-state lithium metal batteries

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Science China chemistry 2025年

作者： Zitian Lin Sucheng Liu Ce Cui Wuhua Liu Yufeng Su Huiyu Song Li Du Jianqiang Hu Zhiming Cui Guangdong provincial key laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology

Solid-state polymer electrolytes hold the potential for market application due to the combination of advantageous properties,such as flexibility,ease of processing and low ***,the sluggish ion transport and poor high-voltage stability pose significant challenges for the practical application of polymer-based solid-state lithium metal batteries (SSLMBs).Therefore,the design and development of polymer-based SSLMBs toward fast-charge and high-voltage is of great significance in high-energydensity ***,this review deeply analyzes the mechanism of ion transport and anti-oxidation of polymer-based solidstate ***,we also systematically and comprehensively summarize the factors that affect ionic conductivity and the electrochemical ***,we outline the solution strategies for simultaneously enhancing both ionic conductivity and high-voltage ***,we discuss the main challenges and the future prospects of polymer-based SSLMBs for further *** is hoped that this review can provide both advances and fundamentals to the research community and pave the way for the development of SSLMBs

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