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Effect of the solid electrolyte interphase on lithium-mediated ammonia synthesis by Cryo-electron microscopy

Chemical engineering Journal 2025年 512卷

作者： Meng, Zhaojun Wang, Ke Bai, Haotian Han, Lijun Yang, Zhiwen Liu, Yanrong CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Beijing Key Laboratory of Solid State Battery and Energy Storage Process Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Henan University Zhengzhou450000 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing100049 China Institute of Chemistry Chinese Academy of Sciences Beijing100190 China

Lithium-mediated nitrogen reduction reaction (Li-NRR) is a promising reaction pathway to realize green ammonia production. However, there is a lack of clear understanding on how solid electrolyte interphase (SEI) membranes affects Li-NRR performance. The effects of different lithium salts on the SEI layer were investigated in this work. Among lithium tetrafluoroborate (LiBF4), lithium perchlorate (LiClO4), and lithium trifluoromethanesulfonate (LiOTf), LiOTf showed better ammonia synthesis performance. At 1 bar N2 and −6 mA cm−2 current density, the faraday efficiency (FE) and ammonia production rate reached 16.94 ± 0.67 % and 3.51 ± 0.14 nmol s−1 cm−2, respectively. Conversely, the LiBF4 electrolyte has the lowest NH3 selectivity and rate under identical operating conditions, which are only 2.41 ± 0.16 % and 0.50 ± 0.03 nmol s−1 cm−2. Cryo-electron microscopy reveals the influence of SEI nanostructures and chemical properties on the performance of lithium-mediated electrochemical synthesis of ammonia. The results of Cryo-electron microscopy showed that the SEI membranes of LiOTf electrolyte exhibited a reticular structure, which was favorable for N2 adsorption, while the SEIs of LiClO4 and LiBF4 electrolytes had a lamellar and irregular planar structure, respectively. Molecular dynamics (MD) simulations and density functional theory (DFT) results showed that the LiOTf electrolyte can more easily generate a stable SEI membrane on the electrode surface. These findings highlight the importance of SEI structure in enhancing the reaction process, and thus provide valuable suggestions for the development of artificial SEI with specific structure. © 2025

关键词： Ammonia

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Programming anti-ribozymes to sense trigger RNAs for modulating gene expression in mammalian cells

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Synthetic and Systems Biotechnology 2025年第3期10卷 827-834页

作者： Zhang, Wenhui Zhao, Shi Wang, Mengyuan Lou, Chunbo Xiang, Yanhui Wu, Qiong Center for Cell and Gene Circuit Design CAS Key Laboratory of Quantitative Engineering Biology Shenzhen Institute of Synthetic Biology Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China State Key Laboratory of Green Biomanufacturing MOE Key Lab. Bioinformatics Center for Synthetic and Systems Biology School of Life Sciences Tsinghua University Beijing 100084 China

Synthetic RNA-based switches provide distinctive merits in modulating gene expression. Simple and flexible RNA-based switches are crucial for advancing the field of gene regulation, paving the way for innovative tools that can sense and manipulate cellular processes. In this research, we have developed programmable ribozymes that are capable of suppressing gene expression in response to specific, endogenously expressed trigger RNAs. We engineer ribozymes by introducing upstream antisense sequences (anti-ribozymes) to inhibit the self-cleaving activity of the hammerhead ribozyme and open the expression of the target gene. The trigger RNA is designed to recognize and bind to complementary sequences within the anti-ribozymes, thereby inhibiting their ability to direct protein synthesis. The anti-ribozyme performance is optimized by regulating the essential sequence modules that play a crucial role in determining the specificity and efficiency of the anti-ribozyme's interaction with its trigger RNA. By applying this switch mechanism to various ribozyme designs, we have shown that it is possible to achieve control over gene expression across a wide range of trigger RNAs. By exploiting these programmable anti-ribozymes, we aim to create a powerful tool for controlling gene expression in mammalian cells, which could have important implications for basic research, disease diagnosis, and therapeutic interventions. © 2025 The Authors

关键词： Anti-ribozyme Antisense RNA sequence Gene expression regulation Ribozyme RNA-based switch Trigger RNA sequence

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Shell engineering on mesoporous metal organic frameworks: Beyond microporous restriction in core-shell architecture

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green Chemical engineering 2025年

作者： Shi, Lijuan Sun, Deyun Xu, Hongxue Maqsood, Zunaira Chen, Shangqing Yi, Qun Key Laboratory of Green Chemical Engineering Process of Ministry of Education Hubei Key Lab of Novel Reactor & Green Chemical Technology School of Chemical Engineering and Pharmacy Wuhan Institute of Technology Wuhan430205 China

Core-shell metal organic frameworks (MOFs) have emerged as a promising platform for efficient separation and sensing, benefiting from the sieving effect of the shell and the large storage capacity of the core. However, conventional core-shell MOFs often encounter challenges with compromised pore integrity, which predominantly restricts their design to microporous cores. In this study, a straightforward strategy to construct functional shells on mesoporous MOFs is proposed. By leveraging dynamic imine chemistry, small-molecule amines are assembled into supramolecular polymers and anchored onto the surface of mesoporous MOFs through metal coordination. This approach preserves the mesoporous structure of the core while introducing hydrogen-bonding channels in the shell, facilitating the selective capture and storage of polar gases. The resulting core-shell MOF demonstrates exceptional CO2/N2 selectivity of up to 10,943 and a high CO2 adsorption capacity, enabling the direct production of high-purity CO2 (99.7 vol.%) from humid flue gas in a single breakthrough experiment. Furthermore, this strategy exhibits excellent stability and versatility across various mesoporous MOFs, underscoring its potential for practical industrial gas separation applications. © 2025 Institute of process engineering, Chinese Academy of Sciences.

关键词： Hydrogen bonds

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Tuning Electrode Wettability to Optimize Nanobubble Nucleation and Reaction Rates in Electrochemical Gas-Evolving Reactions

arXiv

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arXiv 2025年

作者： Wang, Zhenlei Yu, Yaxi Qin, Mengkai Jiang, Hao Guo, Zhenjiang Bai, Lu Wang, Limin Zhang, Xiaochun Zhang, Xiangping Liu, Yawei Beijing Key Laboratory of Solid State Battery and Energy Storage Process CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing100049 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Henan University Zhengzhou450000 China

Bubble formation in electrochemical system often hinders reaction efficiency by reducing active surface area and obstructing mass transfer, yet the mechanisms governing their nanoscale nucleation dynamics and impact remains unclear. In this study, we used molecular dynamics simulations to explore nanobubble nucleation and reaction rates during water electrolysis on planar- and nano-electrodes, with systematically tuning electrode wettability through water-electrode and gas-electrode interactions. We identified distinct nucleation regimes: gas layers, surface nanobubbles, bulk nanobubbles, and no nanobubbles, and revealed a volcano-shaped relationship between wettability and reaction rate, where optimal wettability strikes a balance between suppressing bubbles and ensuring sufficient reactant availability to maximize performance. Nanoelectrodes consistently exhibit higher current densities compared to planar electrodes with the same wettability, due to pronounced edge effects. Furthermore, moderate driving forces enhance reaction rates without triggering surface bubble formation, while excessive driving forces induce surface nanobubble nucleation, leading to suppressed reaction rates and complex dynamics driven by bubble growth and detachment. These findings highlight the importance of fine-tuning wettability and reaction driving forces to optimize gas-evolving electrochemical systems at the nanoscale and underscore the need for multiscale simulation frameworks integrating atomic-scale reaction kinetics, nanoscale bubble nucleation, and microscale bubble dynamics to fully understand bubble behavior and its impact on performance. © 2025, CC BY.

关键词： Wetting

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Efficient continuous synthesis of 2-[3-(trifluoromethyl)phenyl]malonic acid,a key intermediate of Triflumezopyrim,coupling with esterification-condensation-hydrolysis

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Chinese Chemical Letters 2025年第1期36卷 234-238页

作者： Yuexiang Liu Xiangqiao Yang Tong Lin Guantian Yang Xiaoyong Xu Bubing Zeng Zhong Li Weiping Zhu Xuhong Qian Shanghai Key Laboratory of Chemical Biology School of PharmacyEast China University of Science and TechnologyShanghai 200237China Shanghai Frontiers Science Center of Optogenetic Techniques for Cexll Metabolism School of PharmacyEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Bioreactor Engineering East China University of Science and TechnologyShanghai 200237China Engineering Research Center of Pharmaceutical Process Chemistry Ministry of EducationSchool of PharmacyEast China University of Science and TechnologyShanghai 200237China Shanghai Key Laboratory of Green Chemistry and Chemical Processes Department of ChemistrySchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200241China

Triflumezopyrim(TFM)is a novel mesoionic pyrido[1,2-α]pyrimidinones insecticide,which acts on nicotinic acetylcholine receptors(n ACh Rs)and has no cross-resistance with other ***,we firstly developed a new continuous flow approach to synthesis 2-[3-(trifluoromethyl)phenyl]malonic acid,a key intermate of TFM,coupling with esterification,condensation,and *** three-step reactions were optimized and transformed into a continuous synthesis mode by three micro reaction *** with the batch mode,the total reaction time and overall separation yield were improved from more than 12 h and 60%to 18 min and 73.38%,*** solvent consumption and waste emission were significantly reduced,which also provides an eco-friendly and efficient potential tool for the development and production of mesoionic pyrido[1,2-α]pyrimidinones insecticide.

关键词： Triflumezopyrim(TFM) 2-[3-(Trifluoromethyl)phenyl]malonic acid Continuous flow synthesis Micro-reactor

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Challenges and Breakthroughs in Single-Atom Catalysts for Electrocatalytic Nitrate Reduction to Ammonia

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ACS Sustainable Chemistry and engineering 2025年第19期13卷 6875-6899页

作者： Wang, Yang Li, Jin Xing, Xiujing Lv, Yaokang Xiong, Wei Lyu, Renliang Li, Hao Key Laboratory of Green Chemical Engineering Process of Ministry of Education School of Chemistry and Environmental Engineering Wuhan Institute of Technology Wuhan430205 China Chemistry Department University of California DavisCA95616 United States College of Chemical Engineering Zhejiang University of Technology Hangzhou310014 China Tohoku University Sendai980-8577 Japan

Single-atom catalysts (SACs) represent a novel category of catalytic materials with substantial potential for the electrocatalytic reduction of nitrate to ammonia (NO3RR). These catalysts possess multiple advantages, such as excellent atom utilization, electrocatalytic activity, and selectivity, along with tunable composition, structure, and unique electronic properties. These features endow them with great significance and wide application in the NO3RR field. Currently, extensive research is being carried out to engineer highly efficient SACs for NO3RR. This perspective elucidates the merits of SACs and their underlying catalytic mechanisms. It enumerates several common SAC preparation methods and characterization techniques, highlighting the crucial role of density functional theory calculations in guiding the design and development of efficient SACs. The recent practical applications of SACs in NO3RR and several strategies for enhancing their performance are also discussed in this perspective. Finally, some insights into future research directions in this vital area are provided. © 2025 American Chemical Society.

关键词： Electrolytic reduction

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Tailoring solvation sheath for rechargeable zinc-ion batteries:Progress and prospect

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Materials Reports(Energy) 2025年第1期5卷 3-18页

作者： Xiaomin Cheng Jing Dong Haifeng Yang Xiang Li Xinyu Zhao Bixian Chen Yongzheng Zhang Meinan Liu Jian Wang Hongzhen Lin i-Lab&CAS Key Laboratory of Nanophotonic Materials and Devices Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou215123China State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai200237China Anhui Provincial Key Laboratory of Green Carbon Chemistry Fuyang Normal UniversityFuyang236037China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning530004China Helmholtz Institute Ulm(HIU) D89081 UlmKarlsruhe Institute of Technology(KIT)D76021 KarlsruheGermany School of Materials Science and Engineering Jiangsu UniversityZhenjiang212013JiangsuChina

Aqueous zinc-metal based batteries(AZMBs)perfectly combine safety,economy and pro-environment,but their performance is arresting limited by the interfacial instability caused by the large desolvation energy barrier of[Zn(H2O)6]^(2+)and the massive release of active water at the electrolyte/electrode *** this review,we briefly outline the solvation structure of zinc ions and the necessity of ***,the variety of strategies to solve these issues,mainly including reorganizing solvation sheath by changing electrolyte environment and accelerating interface desolvation by constructing artificial interfacial layer,are categorically discussed and systematically ***,perspectives and suggestions regarding desolvation theories,interfacial evolution,material design and analysis techniques are proposed to design highly stable zinc anodes.

关键词： Aqueous zinc-metal based batteries Desolvation Electrolyte strategy Interfacial layer

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Effect of sterically hindered amines on the cycling capacity of biphasic absorbents for industrial CO2 capture

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Journal of Environmental Sciences (China) 2025年 157卷 501-510页

作者： Geng, Zanbu Fu, Le Yang, Yang Wang, Yixi Xu, Wenqing Hao, Runlong Zhan, Daoping Zhu, Tingyu CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Innovation Academy for Green Manufacture Chinese Academy of Sciences Beijing100190 China Department of Environmental Science and Engineering North China Electric Power University Baoding 071003 China Wu-Kun Iron & Steel Co. Ltd. Kunming650302 China University of Chinese Academy of Sciences Beijing 100049 China Key Laboratory of Green and High-value Utilization of Salt Lake Resources Chinese Academy of Sciences Xining 810008 China

The biphasic solvent is a promising solution to reduce regeneration energy consumption in CO2 capture. However, most current biphasic solvents suffer from high viscosity and poor desorption of the rich phase. To the issues, a novel pentamethyldiethylenetriamine (PMDETA)-2-amino-2-methyl-1-propanol (AMP)/diethylenetriamine (DETA)-sulfolane biphasic solvent was developed. The mechanism of AMP affecting CO2 recycling capacity was analyzed. By adjusting the ratio of AMP and DETA, the absorption and desorption performance were balanced, and the recycling capacity and renewable energy consumption of the absorbent were improved. For the P2.4A0.8D0.8S2 biphasic solvent, the CO2 loading of the rich phase was 5.87 mol/L, and the proportion of the rich phase volume ratio was 35%, which surpasses most reported biphasic solvents. The viscosity of the absorbent significantly decreased from 527.00 mPa·s to 92.26 mPa·s, attributed to the beneficial effect of AMP. Thermodynamic analysis showed that the biphasic solvent produced a lower regeneration energy consumption of 1.70 GJ/t CO2, which was 57% lower than that of monoethanolamine (MEA). Overall, the PMDETA-AMP/DETA-sulfolane biphasic solvent exhibited cycle capacity, which provided new insights for the designing of biphasic solvent. © 2024

关键词： Absorption Amines Biphasic absorbent CO2 capture Viscosity

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Quaternary Ammonium Cof-Based Proton Exchange Membranes for Enhanced Electrochemical Hydrogen Compression

SSRN

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SSRN 2025年

作者： Pang, Xiao Liu, Ziwen Xu, Shuting Lv, Kexin Shi, Benbing Dong, Xu Xing, Na Gao, Zhong Zhu, Shiyi Zhang, Leilang Yao, Zengguang Cheng, Lijuan Wang, Hui Xu, Kai Liu, Yawei Wu, Hong Jiang, Zhongyi Key Laboratory for Green Chemical Technology Ministry of Education School of Chemical Engineering and Technology Tianjin University Tianjin300072 China Ningbo Key Laboratory of Green Petrochemical Carbon Emission Reduction Technology and Equipment Zhejiang Institute Tianjin University Zhejiang Ningbo315201 China State Key Laboratory of Synthetic Biology Tianjin University Tianjin300072 China Beijing Key Laboratory of Ionic LiquidsClean Process CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China MOE Key Laboratory of Bioorganic NST Phosphorous Chemistry and Chemical Biology Department of Chemistry Tsinghua University Beijing100084 China

Proton exchange membranes (PEMs) with high proton conductivity, excellent mechanical strength, and minimal hydrogen crossover are crucial for the practical implementation of electrochemical hydrogen energy conversion devices, including electrochemical hydrogen compression (EHC). Herein, hydrazone-linked ionic covalent organic frameworks (iCOF) bearing quaternary ammonium (QA) groups were synthesized and introduced into the sulfonated poly (ether ether ketone) (SPEEK) matrix to fabricate hybrid PEMs. Among them, the orderly arrangement of QA and -NH- groups on iCOF not only rearranged the distribution of -SO3H groups in the SPEEK polymer matrix, increasing the continuity and connectivity of the proton conduction pathways but also formed acid-base pairs with -SO3H groups to facilitate proton dissociation. Additionally, the electrostatic and hydrogen bonding interactions formed between iCOF and SPEEK matrix optimized the microphase separation structure and enhanced the mechanical stability of membranes. As a result, the hybrid PEMs exhibited an enhanced proton conductivity of 469.0 mS cm-1 (80°C, 100% RH) with only 2 wt% iCOF content, high mechanical strength of 91.3 MPa, and superior EHC performance with a high outlet pressure of 3.31 MPa (30°C, 100% RH) and high-purity hydrogen (>99.9%) from a 40% hydrogen-nitrogen mixture. © 2025, The Authors. All rights reserved.

关键词： Hydrogen bonds

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Flotation separation of fluorite from calcite and quartz using 1-hydroxyoctane-1,1-bisphosphonic acid

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Journal of Molecular Liquids 2025年 424卷

作者： Xu, Wei Chen, Fangfang Zhang, Min Jiang, Feng Wang, Jiaming Zhang, Wenjing Peng, Guan Li, Jing Hu, Kang Yu, Hongdong School of Rare Earths University of Science and Technology of China Hefei230026 China Key Laboratory of Rare Earths Ganjiang Innovation Academy Chinese Academy of Sciences Ganzhou341119 China CAS Key Laboratory of Green Process and Engineering National Engineering Research Center of Green Recycling for Strategic Metal Resources Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Baogang Group Mining Research Institute Co. Ltd. Baotou014000 China

Sodium oleate (NaOl) is commonly regarded as a kind of collector with strong recovery ability for fluorite flotation. However, its limited selectivity for fluorite and gangue had affected the production of higher-grade fluorite. In this investigation, 1-hydroxyoctane-1,1-bisphosphonic acid (HOBA) was employed as a potential alternative, offering greater efficiency. Micro-floatation experiments confirmed that HOBA could offer better selectivity than NaOl. Moreover, the interaction mechanisms between HOBA or NaOl and the mineral surfaces of fluorite, calcite, and quartz were systematically studied during the flotation process. Contact angle, zeta potential analyses revealed stronger adsorption on fluorite by HOBA compared to calcite and quartz, which can be attributed to its superior selectivity. FTIR and XPS analyses indicate that this selectivity arises from the chemisorption of reagents on fluorite. DFT calculations further demonstrated that HOBA exhibited the stronger selective adsorption on fluorite than that on calcite and quartz surfaces compared to NaOl, due to its more binding sites, supporting IR and XPS results. Additionally, the electronic structure analysis implies that HOBA should is likely bonded to the mineral surfaces through chemisorption as ionic bonds. © 2025

关键词： Quartz

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