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The reformation of catalyst:From a trial-and-error synthesis to rational design

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Nano Research 2024年第4期17卷 3261-3301页

作者： Ligang Wang Jiabin Wu Shunwu Wang Huan Liu Yao Wang Dingsheng Wang department of chemistry Tsinghua UniversityBeijing 100084China

The appropriate catalysts can accelerate the reaction rate and effectively boost the efficient conversion of various molecules,which is of great importance in the study of chemistry,chemical industry,energy,materials and environmental ***,efficient,environmentally friendly,and easy to operate synthesis methods have been used to prepare various types of *** previous studies have reported the synthesis and characterization of the aforementioned catalysts,more still remain in trial and error methods,without in-depth consideration and improvement of traditional synthesis ***,we comprehensively summarize and compare the preparation methods of the trial-and-error synthesis strategy,structure–activity relationships and density functional theory(DFT)guided catalysts rational design for nanomaterials and atomically dispersed *** also discuss in detail the utilization of the nanomaterials and single atom catalysts for converting small molecules(H_(2)O,O_(2),CO_(2),N_(2),etc.)into value-added products driven by electrocatalysis,photocatalysis,and ***,the challenges and outlooks of mass preparation and production of efficient and green catalysts through conventional trial and error synthesis and DFT theory are featured in accordance with its current development.

关键词： trial-and-error synthesis structure–activity relationships density functional theory(DFT)guidance nanomaterials atomically dispersed catalysts

A Simple-Prepared and Multi-Reusable Adhesive Based on Epoxy Vitrimer

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Chinese Journal of Polymer Science 2024年第10期42卷 1589-1594页

作者： Yu-Ting Wang Huan Liang Yen Wei Jian-Long Wang Xiang-Ming He Yang Yang Institute of Nuclear and New Energy Technology Tsinghua University The Key Laboratory of Bioorganic Phosphorus chemistry & Chemical Biology (Ministry of Education) Department of Chemistry Tsinghua University

Adhesives play an important role in modern society's production and daily life. Developing robust and sustainable adhesives remains a great challenge. Here we report a sustainable epoxy-vitrimer adhesive with high adhesive strength (about 10 MPa) and reusability (82%strength after 3 times). This adhesive can be fabricated from commercially available products through a straightforward hot-pressing method without the need of solvents. The adhesive process is also simple, requiring only 30 min at 180°C. In addition, the vitrimer adhesive has the advantages of both erasability for reuse and excellent water resistance. This work provides a facile strategy to fabricate high-strength adhesive that ensures reusability, recyclability, low cost of raw materials, and simple processing technology. Simultaneously, it expands the range of potential applications for epoxy vitrimers.

关键词： Adhesive Epoxy Reusable Sustainable Vitrimer

Interface matters: how to print single atoms?

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Science China Materials 2024年第3期67卷 1002-1003页

作者： Dingsheng Wang department of chemistry Tsinghua UniversityBeijing 100084China

Recently, single-atom catalysts (SACs) have emerged as highly efficient catalysts for multiple reactions, making them as the new stars in the catalytic field [1–7]. Single metal atoms can be anchored onto various supports (such as defective carbon, oxides, sulfides and carbides [8]), endowing single atoms with diverse electronic and coordination structures.

关键词： sulfide coordination oxides

Electrochemical reduction of carbon dioxide to produce formic acid coupled with oxidative conversion of biomass

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Journal of Energy chemistry 2024年第5期92卷 705-729页

作者： Xi Liu Yifan Wang Zhiwei Dai Daihong Gao Xuebing Zhao Key Laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Institute of Applied chemistry Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon *** is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical *** is the most abundant renewable resource in the natural *** biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon *** this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added ***-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction ***-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis *** was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.

关键词： Electrochemical reduction of CO_(2) Formic acid Oxidative conversion of biomass Lignocellulose Coupled system

Constrained reinforcement learning with statewise projection: a control barrier function approach

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Science China(Information Sciences) 2024年第3期67卷 136-154页

作者： Xinze JIN Kuo LI Qingshan JIA department of Automation tsinghua university

Safety is a critical issue for reinforcement learning(RL), as it may be risky for some actual applications if the learning process involves unsafe exploration. Instead of formulating constraints as expectationbased in constrained RL, considering statewise safety in constrained RL is more meaningful. This work aims to address the issue of safe projection in RL by introducing a control barrier function that inherently learns a safe policy through a set certificate. We seek to analyze some theoretical properties of safe projection in the learning process, including convergence and performance bound, and extend the discussion into ensembles and guided controllers. Moreover, we approach analytical solutions for deterministic and stochastic system dynamics. Experimental results in different tasks show that the proposed method achieves better effects in terms of both performance and safety.

关键词： reinforcement learning safe projection control barrier function

Hydrogen bond-bridged phosphorene flexible film for photodynamic inhibiting Staphylococcus aureus

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Nano Research 2024年第6期17卷 5461-5468页

作者： Ziyu Wei Wenting Li Zhifang Liu Yongfa Zhu Huaqiang Cao department of chemistry Engineering Research Center of Advanced Rare Earth MaterialsTsinghua UniversityBeijing 100084China

Antibiotics are a widely used and effective treatment for bacterial ***,bacteria can gradually evolve during infection,leading to developing resistance to antibiotics,which renders previously effective treatments *** a useful and convenient manner to treat bacterial infections is a great ***,we report a flexible hydrogen-bond-bridged phosphorene film with photodynamic antibacterial properties and excellent mechanical properties,fabricated from electrochemical exfoliation of black phosphorus(BP).When illuminated under 700 nm light,the hydrogen bond-bridged phosphorene flexible film is capable of converting ground-state triplet oxygen(O_(2))into excited-state singlet oxygen(^(1)O_(2)),destroying the structure of the membrane of Staphylococcus aureus,and eventually leading to bacterial death,via breaking the C=C of unsaturated fatty acids within the bacterial cell membrane after the reaction between^(1)O_(2)and unsaturated fatty acids,thus realizing a highly efficient antibacterial approach,which is supported by gas chromatography-mass spectrometry(GC-MS)*** work establishes an effective phototherapy platform for treating bacterial traumatic infections.

关键词： hydrogen bond-bridged phosphorene flexible film photodynamic Staphylococcus aureus

Recent progress in MOFs-based nanozymes for biosensing

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Nano Research 2024年第1期17卷 39-64页

作者： Imamdin Chandio Yongjian Ai Lei Wu Qionglin Liang MOE Key Laboratory of Bioorganic Phosphorus chemistry&Chemical Biology Department of ChemistryLaboratory of Flexible Electronics TechnologyCenter for Synthetic and Systems BiologyTsinghua University-Peking University Joint Centre for Life SciencesTsinghua UniversityBeijing 100084China

Nanozymes are nanomaterials with enzyme-mimicking catalytic *** to natural enzymes,nanozymes show various properties such as easy to manufacture,stable,adjustable,and *** play key roles in biosensing,biocatalysis,and disease *** an important kind of nanozymes,metal-organic framework(MOF)-based nanozymes are receiving a lot of attention due to their structural properties and *** developing MOF with enzymes-like catalytic properties has opened new perspectives in *** review summarizes the up-to-date developments in synthesizing two-dimensional and three-dimensional MOF-based nanozymes and their applications in ***,classification of nanozymes obtained by MOFs is categorized,and different properties of MOF-based nanozymes are ***,the distinctive applications of MOF-based nanozymes in identifying various analytes are thoroughly ***,the recent challenges and progressive directions in this area are highlighted.

关键词： metal-organic frameworks nanozymes metal-organic framework (MOF)-based nanozymes biosensing analytes

Synthesis of uniform two-dimensional MoS_(2) films via thermal evaporation

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Nano Research 2024年第4期17卷 3217-3223页

作者： Xue-Wei Lu Zhewei Li Chen-Kai Yang Weijia Mou Liying Jiao Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China

Two-dimensional(2D)molybdenum disulfide(MoS_(2))holds great potential for various applications such as electronic devices,catalysis,lubrication,anti-corrosion and so *** evaporation is a versatile thin film deposition technique,however,the conventional thermal evaporation techniques face challenges in producing uniform thin films of MoS_(2) due to its high melting temperature of 1375℃.As a result,only thick and rough MoS_(2) films can be obtained using these *** address this issue,we have designed a vacuum thermal evaporation system specifically for large-scale preparation of MoS_(2) thin *** using K2MoS4 as the precursor,we achieved reliable deposition of uniform polycrystalline MoS_(2) thin films with a size of 50 mm×50 mm and controllable thickness ranging from 0.8 to 2.4 *** approach also allows for patterned deposition of MoS_(2) using shadow masks and sequential deposition of MoS_(2) and tungsten disulfide(WS_(2)),similar to conventional thermal evaporation ***,we have demonstrated the potential applications of the obtained MoS_(2) thin films in field effect transistors(FETs),memristors and electrocatalysts for hydrogen evolution reaction(HER).

关键词： thermal evaporation molybdenum disulfide two-dimensional memristors hydrogen evolution reaction

Proposal for a realtime Einstein-synchronization-defined satellite virtual clock

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Chinese Physics B 2024年第7期33卷 268-276页

作者：严晨皓汤雪逸王时光孟李皎悦孙海媛何奕彬王力军 department of Precision Instrument Tsinghua UniversityBeijing 100091China department of Physics Tsinghua UniversityBeijing 100091China

Realization of high performance satellite onboard clock is vital for various positioning, navigation, and timing applications. For further improvement of the synchronization-based satellite time and frequency references, we propose a geosynchronous(GEO) satellite virtual clock concept based on ground–satellite synchronization and present a beacon transponder structure for its implementation(scheduled for launch in 2025), which does not require atomic clocks to be mounted on the satellite. Its high performance relies only on minor modifications to the existing transponder structure of GEO satellites. We carefully model the carrier phase link and analyze the factors causing link asymmetry within the special relativity. Considering that performance of such synchronization-based satellite clocks is primarily limited by the link's random phase noise, which cannot be adequately modeled, we design a closed-loop experiment based on commercial GEO satellites for pre-evaluation. This experiment aims at extracting the zero-means random part of the ground-satellite Ku-band carrier phase via a feedback loop. Ultimately, we obtain a 1σ value of 0.633 ps(two-way link), following the Gaussian distribution. From this result, we conclude that the proposed real-time Einstein-synchronization-defined satellite virtual clock can achieve picosecond-level replication of onboard time and frequency.

关键词： Einstein synchronization satellite virtual clock geosynchronous satellite carrier phase

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