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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 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 Engineering Lanzhou University School of chemistry and Chemical Engineering Shanghai Jiao Tong University School of Biotechnology and Health Sciences Wuyi University

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 enantioselectivities. Furthermore, density functional theory calculations were applied to explain the possible reaction mechanism.

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阴离子诱导的多色发光质子化腙及其可控的机械及热致变色（英文）

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Science China Materials 2025年第1期 125-131页

作者：钱程谢黎霞刘立杰曹占奇田东杰孙冬冬刘国星郭志前郑昕 Department of applied chemistry Henan Agricultural University School of chemistry and Molecular Engineering East China University of Science and Technology

可控的多色发光材料在生物成像、有机光电器件、生物传感和防伪等领域具有重要应用,但目前仍难以定向开发多色发光材料.为了解决这一问题,本文以腙键为桥连接供电子性的三苯胺和吸电子性的吡啶基团,构建了一系列基于不同阴离子的D–π–...

可控的多色发光材料在生物成像、有机光电器件、生物传感和防伪等领域具有重要应用,但目前仍难以定向开发多色发光材料.为了解决这一问题,本文以腙键为桥连接供电子性的三苯胺和吸电子性的吡啶基团,构建了一系列基于不同阴离子的D–π–A型化合物1a–1d.其中, 1b晶体能够发生力和热致荧光蓝移,从红到黄色发光.相反, 1d晶体能够发生力和热致荧光红移,从绿到橙色发光.结构分析表明, 1b中的阴离子有利于阳离子发光团的刚性平面结构,增强了三苯胺的供电子能力和分子间弱相互作用,使晶态1b具有强红光发射.而1d中的阴离子使三苯胺供体围绕中心氮原子呈锥形结构,降低了三苯胺的供电子能力,使其发绿色荧光.该工作为定向力和热致变色型多色发光材料的开发提供了新的思路.

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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01期 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.

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Enantioselective reductive conjugate alkenylation of α,β-enones with keto alkenyl acetates by nickel catalysis

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Science China chemistry 2025年第01期 157-162页

作者： Rong-De He Yun-Lei Luo Qiu-Quan Pan Qi-Wei Yao Xing-Zhong Shu State Key Laboratory of applied Organic chemistry College of Chemistry and Chemical Engineering Lanzhou University

Reactions involving alkenyl acetates offer cost-effective and environmentally friendly routes for alkene synthesis, yet their asymmetric variant remains elusive. Concurrently, asymmetric conjugate alkenylation predominantly centered on nucleophilic addition using alkenyl–M. This manuscript presents an asymmetric reductive conjugate alkenylation reaction involving alkenyl acetates. The method facilitates the enantioselective addition of keto alkenyl groups to α,β-enones, resulting in the formation of unsaturated diketones—a class of useful structural motifs that are challenging to access otherwise. The use of electron-rich Pyroxy ligand is essential for achieving both high reaction efficiency and enantioselectivity.

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Efficient and simple synthesis of B_(2)O_(3)-Al_(2)O_(3)nanocomposites assisted by deep eutectic solvent for production of 5-hydroxymethylfurfural from glucose

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Nano Research 2025年第1期18卷 236-248页

作者： Yuchen Wang Kai Rong Shanlei Chang Youxing Fang Shaojun Dong State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China College of chemistry Jilin UniversityChangchun 130012China

The catalytic conversion of glucose to high valueadded platform chemical 5-hydroxymethylfurfural(HMF)is a promising biorefinery process,and alumina-boria catalysts are considered to be green and mild solid acid catalysts for this catalytic ***,compared to the common synthesis methods with complicated steps,we reported a simple and efficient strategy to prepare B_(2)O_(3)-Al_(2)O_(3)nanocomposites by calcining cost-effective glucose-urea deep eutectic solvent(DES)solution containing the *** prepared B_(2)O_(3)-Al_(2)O_(3)nanocomposites exhibited an open three-dimensional skeleton and two-dimensional porous lamellar substructure,endowing them with a high specific surface area(228.27 m2/g).The introduction of boron changed the ratios of different aluminum species(AlⅣ,AlⅤ,and AlⅥ)and borate species(BO3 and BO4),thus further affecting the acidity and the types of acid sites of the *** prepared B_(2)O_(3)-Al_(2)O_(3)bifunctional acid catalysts possessing abundant Lewis acid sites and adjustable Brønsted acid sites showed complete glucose conversion and 55.38%of HMF yield under the optimum *** study proposed a concise method to synthesize alumina-boria solid acid catalysts assisted by glucose-urea *** hope to extend the application and prospect of this efficient and simple synthesis strategy.

关键词： 5-hydroxymethylfurfural(HMF) deep eutectic solvent glucose alumina-boria acid catalyst

Establishing a new testing protocol of the electrochemical stability window for electric double-layer capacitors

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Science China chemistry 2025年第01期 217-225页

作者： Ruilin Hou Xiaoxi Zhao Tingting Liang Qingyun Dou Shan Xu Xingbin Yan School of Materials Science and Engineering Sun Yat-sen University Laboratory of Clean Energy chemistry and Materials Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of Engineering and applied Sciences Nanjing University Center of Industrial Analysis and Testing Guangdong Academy of Science

The electrochemical stability window(ESW) is crucial for determining the energy density of electric double-layer capacitors(EDLCs). However, current ESW testing protocols of EDLCs are strongly affected by artificial factors, thereby leading to unreliable result. To solve this problem, we first identify the key shortcomings of the traditional protocols by analyzing their test principles. Subsequently, taking an aqueous carbon-based EDLC as an example, we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods. With the aid of this descriptor, we propose a new ESW testing protocol, which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations. The protocol can be extended from the single electrode to the full device. This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.

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Small modifications of endo-functionalized cavities lead to large changes in molecular interaction in water

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Science China chemistry 2025年第1期 369-376页

作者： Song-Meng Wang Hao Nian Yan-Fang Wang Li-Shuo Zheng Yu-Tao Zheng Yi-Wei Dong Liping Huang Xiaoping Wang Wei Jiang Liu-Pan Yang Department of chemistry Southern University of Science and Technology School of chemistry and Pharmaceutical Sciences State Key Laboratory for Chemistry and Molecular Engineering of Medicinal ResourcesGuangxi Normal University School of Pharmaceutical Science Hengyang Medical School University of South China

Studying molecular recognition in aqueous environments is crucial for understanding biological processes. Herein, we present a series of N-doped endo-functionalized anthracene-based cavities by introducing inward-directed pyridine units. The subtle modifications can significantly affect the binding properties of these receptors, which is similar to the mutations in biological systems. Combining theoretical calculations and molecular recognition experiments demonstrated that these “mutations” have an impact on the hydrophobicity and charge distribution of the hosts, consequently significantly influencing molecular *** is crucial for understanding the intricate mechanisms of molecular-level interactions in biological receptors.

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通过Knoevenagel缩合双酮吡咯和吲哚二噻吩得到乙烯基链接的非晶态共轭聚合物并应用于柔性晶体管（英文）

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Science China Materials 2025年第1期 110-116页

作者：陈雁琳陈品宇周仕弘杨志伟龙海军梁先峰陈天文黎静谭陆西张浩力董立春刘子桐 School of chemistry and Chemical Engineering Chongqing University State Key Laboratory of applied Organic chemistry (SKLAOC) Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University Chongqing institute of Green and Intelligent Technology Chinese Academy of Sciences

共轭聚合物在柔性薄膜晶体管器件中展现出广泛的应用潜力.然而,设计和合成具有高迁移率与优良弯曲（或拉伸）稳定性的共轭聚合物仍面临诸多挑战.本文报道了一种具有乙烯基链接的共轭聚合物PDPPVIDT,该聚合物通过双侧甲基取代的双酮吡咯...

共轭聚合物在柔性薄膜晶体管器件中展现出广泛的应用潜力.然而,设计和合成具有高迁移率与优良弯曲（或拉伸）稳定性的共轭聚合物仍面临诸多挑战.本文报道了一种具有乙烯基链接的共轭聚合物PDPPVIDT,该聚合物通过双侧甲基取代的双酮吡咯（DPP）和茚并二噻吩（IDT）二醛单体,采用环境友好的Knoevenagel缩合反应合成.该反应条件温和,且具备良好的环境友好性及规模化潜力.研究结果表明,聚合物主链的平面性得以增强,并且显示出稳定的π-π堆积特性.此外,由于乙烯基的构象异构化特性, PDPPVIDT薄膜呈现出近乎无定形的特性,从而同时确保了电荷传输效率与柔韧性.基于PDPPVIDT的柔性有机薄膜晶体管（OTFT）器件展示出高达1.70 cm2V-1s-1的优异迁移率和良好的机械弯曲恢复能力.该研究展示了乙烯基链接D-A共轭聚合物的潜力,并强调了其生产过程的工业适应性,为未来柔性电子材料的设计与合成提供了新的思路.

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Endogenous/exogenous dual stimulation“ROS engineering”amplification combined with autophagy-augmented for efficient ferroptosis therapy

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Nano Research 2025年第1期18卷 597-606页

作者： Pengye Du Pengpeng Lei Yuan Liang Ran An Yi Wei Shuyu Liu Jianhao Zheng Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Department of chemistry Tsinghua UniversityBeijing 100084China

“Reactive oxygen species(ROS)engineering”is one of the most promising anti-tumor treatments developed in recent *** explosion of ROS will cause oxidative stress,thereby inducing tumor cell ***,ROS accumulation in tumor cells is eliminated by endogenous cellular self-regulation *** this work,a kind of endogenous/exogenous dual stimulation nanoagent noted as UMZC is *** reaction occurs between NH_(2)-MIL-88B(Fe)contained in UMZC and the overexpression of endogenous H_(2)O_(2)to generate ROS,amplified by endogenous H_(2)S of colon tumor *** addition,NH_(2)-MIL-88B(Fe)also functions to deplete glutathione(GSH)for stopping it from consuming *** nanoparticles at the core of UMZC convert near-infrared into visible light,which excites zinc phthalocyanine to initiate the photochemical reaction that generates more ROS,thus alleviating the lack of tissue penetration depth for visible *** agonist chitosan oligosaccharides induce enhancement of cellular autophagy for disrupting cellular metabolic stress and the resistance to oxidative stress of tumor cells,allowing“ROS engineering”to fully exert anti-tumor *** of ROS generation,GSH depletion,and induced cellular autophagy caused by nanoagents have promoting effects on the occurrence of ***,the nanoagents show the ability to effectively treat colon tumors.

关键词： reactive oxygen species(ROS)engineering upconversion nanoparticles cellular autophagy ferroptosis tumor therapy