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Highly Porous Yet Transparent Mechanically Flexible Aerogels Realizing Solar-Thermal Regulatory Cooling

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Nano-Micro Letters 2024年第7期16卷 231-243页

作者： Meng Lian Wei Ding Song Liu Yufeng Wang Tianyi Zhu Yue-EMiao Chao Zhang Tianxi Liu State Key Laboratory for Modification of chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620People’s Republic of China Key Laboratory of synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122People’s Republic of China

The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.

关键词： Transparent aerogel Cellulose nanofiber aerogel Delaminated gelation Thermal insulation Passive daytime radiative cooling

Rational surface charge engineering of haloalkane dehalogenase for boosting the enzymatic performance in organic solvent solutions

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Chinese Journal of chemical Engineering 2024年第1期65卷 276-285页

作者： Yin Wu Yan Sun Department of Biochemical Engineering School of Chemical Engineering and Technology and Key Laboratory of Systems Bioengineering and Frontiers Science Center for Synthetic Biology(Ministry of Education)Tianjin UniversityTianjin 300350China

Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.

关键词： Surface charge engineering Organic solvent resistance Molecular dynamics simulation Haloalkane dehalogenase

Progress and prospects of chiral nanomaterials for biosensing platforms

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Rare Metals 2024年第6期43卷 2469-2497页

作者： Yu-Cheng Ouyang Bong-Jun Yeom Yuan Zhao Wei Ma School of Food Science and Technology State Key Laboratory of Food Science and ResourcesJiangnan University Key Laboratory of synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan University Department of chemical Engineering Hanyang University

Chiral nanomaterials have distinct chiroptical properties of preferential interactions to circularly polarized lights.Chirality-based biosensors have emerged for detection of biomolecules,ions and cells in recent years.This review provides an extensive overview of biosensors based on chiral nanomaterials,starting with approaches to chiral nanomaterials construction in terms of fabrication strategies.Fabrication of chiral nanomaterials and their biosensor applications is presented for different material types,with special emphasis on the role and importance of material properties and signal generation in detection.We assessed the technological prospects of the emerging fields of chiral construction,circularly polarized luminescence,Raman optical activity and so on along with their current challenges.Prospective venues for future research on chiral nanomaterials in fabrication,biosensing,disease diagnosis and treatment are also presented in the review.

关键词： Chiral nanomaterials Circular dichroism Biosensors

A Radiative-Cooling Hierarchical Aligned Porous Poly(vinylidene fluoride)Film by Freeze-Thaw-Promoted Nonsolvent-Induced Phase Separation

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Chinese Journal of Polymer Science 2024年第7期42卷 976-983,I0009页

作者： Yiting Zhang Jiahui Sun Yufeng Wang Yunchen Wu Chun Huang Chao Zhang Tianxi Liu Key Laboratory of synthetic and Biological Colloids Ministry of Education School of Chemical and Material EngineeringJiangnan UniversityWuxi214122China State Key Laboratory for Modification of chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China

Passive daytime radiative cooling(PDRC)is an innovative and sustainable cooling technology that holds immense potential for addressing the energy crisis.Despite the numerous reports on radiative coolers,the design of a straightforward,efficient,and readily producible system remains a challenge.Herein,we present the development of a hierarchical aligned porous poly(vinylidene fluoride)(HAP-PVDF)film through a freeze-thaw-promoted nonsolvent-induced phase separation strategy.This film features oriented microporous arrays in conjunction with random nanopores,enabling efficient radiative cooling performance under direct sunlight conditions.The incorporation of both micro-and nano-pores in the HAP-PVDF film results in a remarkable solar reflectance of 97%and a sufficiently high infrared thermal emissivity of 96%,facilitating sub-environmental cooling at 18.3℃ on sunny days and 13.1℃ on cloudy days.Additionally,the HAP-PVDF film also exhibits exceptional flexibility and hydrophobicity.Theoretical calculations further confirm a radiative cooling power of 94.8 W·m^(-2)under a solar intensity of 1000W·m^(-2),demonstrating a performance comparable to the majority of reported radiative coolers.

关键词： Daytime radiative cooling Hierarchical porosity PVDF porous film Thermal insulation Nonsolvent-induced phase separation

Inhibition of Defect-Induced Ice Nucleation, Propagation, and Adhesion by Bioinspired Self-Healing Anti-Icing Coatings

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Research 2024年第1期2023卷 237-246页

作者： Shu Tian Ruiqi Li Xinmeng Liu Jiancheng Wang Junyu Yu Sijia Xu Yunqing Tian Jing Yang Lei Zhang Department of Biochemical Engineering Frontier Science Center for Synthetic Biology and Key Laboratory of Systems Bioengineering(MOE)School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Binzhou Institute of Technology Weiqiao-UCAS Science and Technology ParkBinzhou CityShandong Province 256606China

Anti-icing coatings on outdoor infrastructures inevitably suffer from mechanical injuries in numerous icing scenarios such as hailstorms,sandstorms,impacts of foreign objects,and icing–deicing cycles.Herein,the mechanisms of surface-defect-induced icing are clarified.At the defects,water molecules exhibit stronger adsorption and the heat transfer rate increases,accelerating the condensation of water vapor as well as ice nucleation and propagation.Moreover,the ice–defect interlocking structure increases the ice adhesion strength.Thus,a self-healing(at−20℃)antifreeze-protein(AFP)-inspired anti-icing coating is developed.The coating is based on a design that mimics the ice-binding and non-ice-binding sites in AFPs.It enables the coating to markedly inhibit ice nucleation(nucleation temperature<−29.4℃),prevent ice propagation(propagation rate<0.00048 cm^(2)/s),and reduce ice adhesion on the surface(adhesion strength<38.9 kPa).More importantly,the coating can also autonomously self-heal at−20℃,as a result of multiple dynamic bonds in its structure,to inhibit defect-induced icing processes.The healed coating sustains high anti-icing and deicing performance even under various extreme conditions.This work reveals the in-depth mechanism of defect-induced ice formation as well as adhesion,and proposes a self-healing anti-icing coating for outdoor infrastructures.

关键词： coating defect clarified

Biomimetic MXene membranes with negatively thermo-responsive switchable 2D nanochannels for graded molecular sieving

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Green Energy & Environment 2024年第6期9卷 1058-1067页

作者： Yi Wang Yangyang Wang Chang Liu Dongjian Shi Weifu Dong Baoliang Peng Liangliang Dong Mingqing Chen The Key Laboratory of synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxiJiangsu214122China International Research Center for Photo-responsive Molecules and Materials Jiangnan UniversityWuxiJiangsu214122China Research Institute of Petroleum Exploration&development(RIPED) PetroChina/Key Laboratory of Oilfield ChemistryCNPCBeijing100083China

Negatively thermo-responsive 2D membranes,which mimic the stomatal opening/closing of plants,have drawn substantial interest for tunable molecular separation processes.However,these membranes are still restricted significantly on account of low water permeability and poor dynamic tunability of 2D nanochannels under temperature stimulation.Here,we present a biomimetic negatively thermo-responsive MXene membrane by covalently grafting poly(N-isopropylacrylamide)(PNIPAm)onto MXene nanosheets.The uniformly grafted PNIPAm polymer chains can enlarge the interlayer spacings for increasing water permeability while also allowing more tunability of 2D nanochannels for enhancing the capability of gradually separating multiple molecules of different sizes.As expected,the constructed membrane exhibits ultrahigh water permeance of 95.6 L m^(-2) h^(-1) bar^(-1) at 25℃,which is eight-fold higher than the state-of-the-art negatively thermoresponsive 2D membranes.Moreover,the highly temperature-tunable 2D nanochannels enable the constructed membrane to perform excellent graded molecular sieving for dye-and antibiotic-based ternary mixtures.This strategy provides new perspectives in engineering smart 2D membrane and expands the scope of temperature-responsive membranes,showing promising applications in micro/nanofluidics and molecular separation.

关键词： Thermo-responsive 2D membrane MXene nanosheets PNIPAm Temperature-tunable 2D nanochannels Graded molecular sieving

Controlling hydrogenation of C=C and C=O bonds in cinnamaldehyde using Pt1/Ni and Pt1/Co single-atom alloy catalysts

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Rare Metals 2024年第6期43卷 2859-2868页

作者： Huan-Shi Lan Yi-Da Yang Qing-Di Sun Hao Zhang Ying Zhang Qian He Ran Chen Guo-Yi Bai Xiao-Hui He Hong-Bing Ji School of Chemistry and chemical Engineering Guangxi University Key Laboratory of Bioinorganicand synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen University UBFC CNRSENSMMFEMTO-ST Institute College of Chemistry and Materials Science Hebei University State Key Laboratory Breeding Base of Green-chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of Technology

Selective hydrogenation of C=C and C=O bonds in cinnamaldehyde (CAL) to produce desired products is a challenging task due to the complex conjugate system of the two unsaturated functional groups.In this study,a simple ball milling method is presented for synthesizing Pt-based single-atom alloy catalysts (SAAs) that can function as a control switch for the selective hydrogenation of CAL into highly valuable products.

关键词： SELECTIVE HYDROGENATION CHEMOSELECTIVE HYDROGENATION NANOPARTICLES GENERATION EFFICIENT FE CO

Hybridization chain reaction-based DNA nanomaterials for biosensing,bioimaging and therapeutics

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Chinese chemical Letters 2024年第2期35卷 223-231页

作者： Zhaoyue Lv Mengxue Huang Peiran Li Mengdi Xu Chi Yao Dayong Yang Frontiers Science Center for synthetic Biology Key Laboratory of Systems Bioengineering (MOE)Institute of Biomolecular and Biomedical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Zhejiang Institute of Tianjin University Ningbo 315201China

DNA nanomaterials hold great promise in biomedical fields due to its excellent sequence programmability,molecular recognition ability and biocompatibility.Hybridization chain reaction(HCR)is a simple and efficient isothermal enzyme-free amplification strategy of DNA,generating nicked double helices with repeated units.Through the design of HCR hairpins,multiple nanomaterials with desired functions are assembled by DNA,exhibiting great potential in biomedical applications.Herein,the recent progress of HCR-based DNA nanomaterials for biosensing,bioimaging and therapeutics are summarized.Representative works are exemplified to demonstrate how HCR-based DNA nanomaterials are designed and constructed.The challenges and prospects of the development of HCR-based DNA nanomaterials are discussed.We envision that rationally designing HCR-based DNA nanomaterials will facilitate the development of biomedical applications.

关键词： DNA nanotechnology Hybridization chain reaction DNA nanomaterials Biosensing Bioimaging Therapeutics

Regulation of interlayer channels of graphene oxide nanosheets in ultra-thin Pebax mixed-matrix membranes for CO_(2) capture

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Chinese Journal of chemical Engineering 2024年第3期67卷 257-267页

作者： Feifan Yang Yuanhang Jin Jiangying Liu Haipeng Zhu Rong Xu Fenjuan Xiangli Gongping Liu Wanqin Jin State Key Laboratory of Materials-Oriented chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Shandong Production and Research Long Membrane Technology development Co. Ltd.Yantai Economic Development ZoneYantai 265505China

For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(MMMs)incorporated by graphene oxide(GO),in which the interlayer channels were regulated to optimize the CO_(2)/N_(2) separation performance.Various membrane preparation conditions were systematically investigated on the influence of the membrane structure and separation performance,including the lateral size of GO nanosheets,GO loading,thermal reduction temperature,and time.The results demonstrated that the precisely regulated interlayer channel of GO nanosheets can rapidly provide CO_(2)-selective transport channels due to the synergetic effects of size sieving and preferential adsorption.The GO/Pebax ultra-thin MMMs exhibited CO_(2)/N_(2) selectivity of 72 and CO_(2) permeance of 400 GPU(1 GPU=106 cm^(3)(STP)·cm^(2)·s^(-1)·cmHg^(-1)),providing a promising candidate for CO_(2) capture.

关键词： Mixed-matrix membrane Ultra-thin membrane Pebax Graphene oxide CO_(2) capture