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Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China chemistry 2025年第1期68卷 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State Key Laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green Catalysis center College of Chemistry Zhengzhou University State Key Laboratory of Natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-C(sp3)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory(DFT) calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET) mechanism.

关键词： gold catalysis peptide alkylation C-C coupling radical

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Efficient photocatalytic reduction of CO2 to formate by a molecular noble metal-free system

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Science China chemistry 2025年第1期68卷 152-156页

作者： Lihua Zhang Lingjing Chen Huatian Shi Yue Wei Gui Chen Tai-Chu Lau School of Environment and Civil Engineering Research Center for Eco-environmental Engineering Dongguan University of Technology Department of chemistry and Institute of Molecular Functional Materials City University of Hong Kong

Reducing CO2to carbon-neutral solar fuels can not only alleviate the energy demand but also mitigate the greenhouse *** present,developing an efficient non-noble metal photo/electrocatalytic system for converting CO2to a specific product beyond CO is still a big ***,we report a new cobalt complex bearing 2,2′-bi-1,10-phenanthroline ligand that can photocatalytically reduce CO2to formate （HCOO-）.Turnover number （TON） for HCOO-up to 677 with 99%selectivity can be achieved using organic dyes purpurin as photosensitizer and 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole （BIH） as sacrificial reductant in a CO2-saturated NMP/TEA （v/v,3:1） solution under visible light *** potential electrolysis at-1.41 V （***/Ag Cl） in the presence of 12 m M Et3NHBF4also produced HCOO-with Faradaic efficiency of 39%.Spectroscopic and electrochemical studies suggest that a[CoI-H]species is the key intermediate for CO2reduction.

关键词： photocatalysis noble metal-free CO2 reduction formate cobalt hydride

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

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

A low redox potential and long life organic anode material for sodium-ion batteries

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Journal of Energy chemistry 2025年第1期100卷 557-564页

作者： Zhi Li Yang Wei Kang Zhou Xin Huang Xing Zhou Jie Xu Taoyi Kong Junwei Lucas Bao Xiaoli Dong Yonggang Wang Department of chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Institute of New Energy Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) Fudan University Department of chemistry Boston College School of Materials Science and Engineering Anhui University of Technology

Sodium-ion batteries （SIBs） with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ***,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials（>1 V）.Organic electrodes with low redox potential that can be used as anode are ***,a novel organic anode material （tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na4TDC） has been developed with low redox potential （<0.7 V） and excellent cyclic *** three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per ***,the Na4TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg *** pairing with a thick Na3V2（PO4）3cathode (20.6 mg cm-2),the as-fabricated full cell exhibited high operating voltage （2.8 V）,excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na4TDC anode material for SIBs.

关键词： Organic anode material Low redox potential Composite anode Sodium-ion batteries

Computational protein design and structure prediction—the 2024Nobel prize in chemistry

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Science China chemistry 2025年

作者： Peilong Lu Lei Liu School of Life Sciences and research center for Industries of the Future Westlake University Tsinghua-Peking Joint center for Life Sciences Ministry of Education Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology Center for Synthetic and Systems Biology Department of Chemistry Tsinghua University

The 2024 Nobel prize in chemistry recognizes groundbreaking advancements in protein science, highlighting the power of artificial intelligence (AI) to decipher and design the molecular machinery of life. Half of the prize was awarded to David Baker for the computational design of proteins; the other to Demis Hassabis and John Jumper for their AI-driven predictions of protein structures. This article briefly reviews their achievements, and discusses the opportunities and directions that their work has enabled (Figure1).

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Catalytic atroposelective synthesis of indolyl quinazolinones bearing N-N/C-C diaxes

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Science China chemistry 2025年

作者： Ning-Yi Wang Shuo Gao Zhu-Di Shu Bei-Bei Cheng Chun Ma Yu-Chen Zhang Feng Shi research center of Chiral Functional Heterocycles School of Chemistry and Materials Science Jiangsu Normal University School of Petrochemical Engineering Changzhou University School of chemistry and Chemical Engineering Henan Normal University

The first catalytic atroposelective synthesis of indole derivatives bearing N-N/C-C diaxes has been established by the strategy of de novo ring formation. By this strategy, various indolyl quinazolinones bearing vicinal N-N/C-C diaxes were synthesized in high yields with overall good diastereoselectivities and excellent enantioselectivities via chiral phosphoric acid-catalyzed onepot asymmetric formal (5+1) cycloaddition/oxidation reaction. Moreover, such indolyl quinazolinones bearing vicinal N-N/CC diaxes have good configurational stability and could be converted into new chiral ligands with applications in asymmetric catalysis. Therefore, this work not only offered a new member for the family of diaxial atropisomers, but also provided a powerful strategy for catalytic asymmetric synthesis of atropisomers bearing N-N/C-C diaxes.

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Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization

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Science China chemistry 2025年

作者： Yina Nie Weijie Yang Xin Wang Xiang Li Lele Wei Xiaolin Bai Lin Liu Feng Fu Jun Wan College of chemistry & Chemical Engineering Research Institute of Comprehensive Energy Industrial Technology Shaanxi Key Laboratory of Chemical Reaction Engineering Yan'an University Anhui Engineering research center of Carbon Neutrality College of Chemistry and Materials Science Anhui Normal University

The production of ultra-low sulfur clean fuels holds global significance for improving energy efficiency and reducing environmental pollution. Photocatalytic aerobic oxidative desulfurization（PODS） offers an attractive approach to efficiently remove refractory heterocyclic aromatic sulfur compounds under mild conditions. However, the sluggish charge dynamics,insufficient molecule activation, and slow mass transfer within photocatalysts restrict the overall desulfurization efficiency,hindering the widespread application of this technology. Herein, we developed a defective g-C3N4（M1U3CN） photocatalyst with bridged N3Cvacancies and hierarchical porous structures to address these limitations. This catalyst not only demonstrates outstanding dibenzothiophene（DBT） removal efficiency of 99.6% for model oil with high conversion and selectivity but also achieves complete sulfur removal from gasoline as well as 96.7% sulfur removal for distilled diesel at room temperature,successfully achieving ultradeep aerobic oxidative desulfurization. The introduction of rich N3Cvacancies and abundant micromeso-macroporous distribution in M1U3CN enhances kinetic efficiencies by promoting charge carrier separation, mass transfer,and molecular activation simultaneously; resulting in exceptional PODS performance. This work provides a collaborative strategy to overcome kinetic challenges in aerobic oxidative desulfurization via defect and structural engineering of the catalyst.

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Chiral phosphoramidite ligand-modulated palladium auto-tandem catalysis for asymmetric dehydrogenative dienylation of imines with α-alkenes

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Science China chemistry 2025年

作者： Zhong-Sheng Nong Hao-Fan Qian Ying-Chun Chen Pu-Sheng Wang Liu-Zhu Gong Hefei National research center for Physical Sciences at the Microscale and Department of chemistry University of Science and Technology of China Key Laboratory of Drug Targeting and Drug Delivery System (Sichuan University) Ministry of Education and Sichuan Research Center for Drug Precision Industrial Technology West China School of Pharmacy Sichuan University School of Materials and chemistry Southwest University of Science and Technology

The development of efficient processes allowing rapid access to complex chiral molecules from easily available alkenes is a long-term pursuit in the synthetic chemistry community. Transition metal-catalyzed asymmetric functionalization of allylic C–H bond represents a unique alternative toward this goal. However, enantioselective dehydrogenative transformation of olefins to value-added optically enriched molecules remains yet to be discovered. Here, we report a highly enantioselective dehydrogenative dienylation of imines with unactivated α-alkenes driven by the synergistic action of palladium complex and carboxylic acid. Chiral phosphoramidite ligands turned out to be superior in modulating the performance of palladium autotandem catalysis and allowed a broad range of α-alkenes and imines to be transformed into chiral dienylamines. Mechanistic studies suggest that the dienes could be in situ generated from α-alkenes through a palladium(0)-mediated dehydrogenative process in the presence of excess benzoquinone oxidants, and then participated in the Pd-chiral phosphoramidite-catalyzed intermolecular vinylogous-type addition to the imines activated by the carboxylic acid co-catalyst. Notably, the second β-H elimination occurring in the dienylation event might be the turnover-limiting step.

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