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"Weakly Adsorbed CO2 and H2O Species on Monoethanolamine Films in a Room-Temperature CO2 and Direct Air Capture Cycle: An In Situ Infrared Study"

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INDUSTRIAL & engineering CHEMISTRY RESEARCH 2024年第10期63卷 4742-4742页

作者： Oduntan, Aderinsola Chuang, Steven S. C. School of Polymer Science and Polymer Engineering Department of Chemical Biomolecular and Corrosion Engineering The University of Akron 200 E Buchtel Commons Akron Ohio 44325-3909 United States

The binding states of adsorbed CO2 species on monoethanolamine (MEA) thin films in a CO2 and direct air capture cycle at 25 °C have been studied by in situ infrared spectroscopy. CO2 adsorption produced two types of adsorbed CO2: (i) hydrogen-bonded ammonium carbamate, as strongly adsorbed CO2, which can only be removed by heating above 25 °C and (ii) carbamic acid, as weakly adsorbed CO2, which can be removed at room temperature from the MEA film. The infrared results suggest that carbamic acid is on an amine site, which is isolated by OH from neighboring MEA molecules and further clarify the sequence of the formation of adsorbed CO2. Weakly adsorbed CO2 and H2O species were observed for the first time on MEA and nonaqueous MEA thin films. Decreasing the concentration of CO2 from 100% to 420 ppm of CO2/1.5% H2O (atmospheric CO2) for direct air capture decreased the CO2 capture capacity and increased the adsorption half-time while the CO2 desorption half-time (i.e., rate) remained at the same level. Controlling the type and structure of adsorbed CO2 could be effective in bringing down the energy needed for the regeneration of amine solvents and sorbents through enhancing the density of amine sites for carbamic acid.

关键词： Adsorption Amines Noncovalent interactions Organic compounds Thin films

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Development of a radical polymerization algorithm for molecular dynamics simulations of antifreezing hydrogels with double-network structures

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npj Computational Materials 2023年第1期9卷 204-213页

作者： Yonglan Liu Dong Zhang Yijing Tang Xiong Gong Jie Zheng Department of Chemical Biomolecularand Corrosion EngineeringThe University of AkronAkronOHUSA School of Polymer Science and Polymer Engineering The University of AkronAkronOHUSA

The development and understanding of antifreezing hydrogels are crucial both in principle and practice for the design and delivery of new *** current antifreezing mechanisms in hydrogels are almost exclusively derived from their incorporation of antifreezing additives,rather than from the inherent properties of the polymers ***,developing a computational model for the independent yet interconnected double-network(DN)structures in hydrogels has proven to be an exceptionally difficult ***,we develop a multiscale simulation platform,integrating‘random walk reactive polymerization’(RWRP)with molecular dynamics(MD)simulations,to computationally construct a physically-chemically linked PVA/PHEAA DN hydrogels from monomers that mimic a radical polymerization and to investigate water structures,dynamics,and interactions confined in PVA/PHEAA hydrogels with various water contents and temperatures,aiming to uncover antifreezing mechanism at atomic *** simulation results indicate that the antifreezing property of PVA/PHEAA hydrogels arises from a combination of intrinsic,strong water-binding networks and crosslinkers and tightly crosslinked and interpenetrating double-network structures,both of which enhance polymer-water interactions for competitively inhibiting ice nucleation and *** computational findings provide atomic-level insights into the interplay between polymers and water molecules in hydrogels,which may determine their resistance to freezing.

关键词： freezing polymerization hydrogel

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Highly conductive and tough double-network hydrogels for smart electronics

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SmartMat 2024年第2期5卷 54-66页

作者： Dong Zhang Yijing Tang Xiong Gong Yung Chang Jie Zheng Department of Chemical Biomolecularand Corrosion EngineeringThe University of AkronAkronOhioUSA School of Polymer Science and Polymer Engineering The University of AkronAkronOhioUSA R&D Center for Membrane Technology and Department of Chemical Engineering Chung Yuan Christian UniversityTaiwanChina

Development and understanding of highly mechanically robust and electronically conducting hydrogels are extremely important for ever-increasing energy-based *** mixing/blending of conductive additives with hydrophilic polymer network prevents both high mechanical strength and electronic conductivity to be presented in polymer ***,we proposed a double-network(DN)engineering strategy to fabricate PVA/PPy DN hydrogels,consisting of a conductive PPy-PA network via in-situ ultrafast gelation and a tough PVA network via a subsequent freezing/thawing *** resultant PVA/PPy hydrogels exhibited superior mechanical and electrochemical properties,including electrical conductivity of~6.8 S/m,mechanical strength of~0.39 MPa,and elastic moduli of~0.1 *** further transformation of PVA/PPy hydrogels into supercapacitors,they demonstrated a high capacitance of~280.7 F/g and a cycle life of 2000 galvanostatic charge/discharge cycles with over 94.3%capacity retention at the current density of 2 mA/cm2 and even subzero temperatures of−20℃.Such enhanced mechanical performance and electronic conductivity of hydrogels are mainly stemmed from a synergistic combination of continuous electrically conductive PPy-PA network and the two interpenetrating DN *** in-situ gelation strategy is applicable to the integration of ionic-/electrical-conductive materials into DN hydrogels for smart-soft electronics,beyond the most commonly used PEDOT:PSS-based hydrogels.

关键词： conducting polymers double-network hydrogels smart electronics supercapacitors

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Bio-inspired Smart Composites with Multi-scale Architecture and Surface engineering 23

Bio-inspired Smart Composites with Multi-scale Architecture ...

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23rd International Conference on Composite Materials, ICCM 2023

作者： Zeng, Songshan Shen, Kuangyu Li, Rui Smith, Andrew Zhang, Dianyun Sun, Luyi Polymer Program Institute of Materials Science Department of Chemical & Biomolecular Engineering University of Connecticut United States

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Harnessing mechanochemical fluorescence toward autonomous damage-reporting coatings

RSC Applied Polymers

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RSC Applied polymers 2025年第3期3卷 592-597页

作者： Wang, Zeyu Zhou, Junfeng Ling, Zichen Zhou, Qixin Wang, Junpeng School of Polymer Science and Polymer Engineering The University of Akron Akron 44325 OH United States Department of Chemical Biomolecular and Corrosion Engineering The University of Akron Akron 44325 OH United States

Protective coatings are essential for shielding engineering materials from environmental and mechanical damage. A significant endeavor in this regard is detecting the damage in coatings and implementing necessary repairs. However, conventional detection methods often require specialized equipment and expertise, rendering them impractical for real-time monitoring. This work introduces an autonomous damage-reporting coating system based on a stress-responsive polymer network containing a Diels-Alder adduct mechanophore. When subjected to mechanical damage, the mechanophore undergoes a retro-Diels-Alder reaction, liberating a fluorescent π-extended anthracene moiety. The mechanically triggered “off-to-on” optical signal allows for highly sensitive detection of material damage preceding failure. A quantitative relationship between the extent of impact damage and the mechanochemically generated fluorescence is established, facilitating the prediction of material failure. Remarkably, the damage-reporting functionality is maintained even after incorporating pigments into the coating formulation, thereby broadening the applicability of this smart coating system in real-world scenarios. © 2025 RSC.

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“One stone,two birds”solvent system to fabricate microcrystalline cellulose–Ti_(3)C_(2)T_(x)nanocomposite film as a flexible dielectric and thermally conductive material

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Nano Research 2023年第2期16卷 3240-3253页

作者： Yong-Zhu Yan Shuwei Li Sung Soo Park Wei-Jin Zhang Jun Seok Lee Jung Rae Kim Dong Gi Seong Chang-Sik Ha Department of Polymer Science and Engineering School of Chemical EngineeringPusan National UniversityBusan 46241Republic of Korea School of Chemical and Biomolecular Engineering Pusan National UniversityBusan 46241Republic of Korea Division of Advanced Materials Engineering Dong-Eui UniversityBusan 47340Republic of Korea

A strategy for fabricating microcrystalline cellulose–Ti_(3)C_(2)T_(x)(MCC–MXene)nanocomposite films with high relative permittivity,high thermal conductivity,and excellent mechanical properties was *** MCC–MXene nanocomposite film was fabricated by casting a solution containing N,N-dimethylacetamide/lithium chloride(DMAc/LiCl)-soluble MCC and DMAcdispersible MXene nanosheets,followed by humidity control *** MXene nanosheets greatly enhanced the permittivity of the nanocomposite films owing to interfacial ***,the nanocomposite film with 20 wt.%MXene content achieved a desirable permittivity of 71.4 at 102 Hz(a 770%improvement against that of neat cellulose),while the dielectric loss only increased by 1.8 times(from 0.39 to 0.70).The obtained nanocomposite films with 20 wt.%and 30 wt.%MXene exhibited remarkable in-plane thermal conductivities of 8.523 and 9.668 W∙m^(−1)∙K^(−1),respectively,owing to the uniform dispersion and selfalignment of the MXene layered ***,the uniformly dispersed MXene nanosheets in the MCC network with interfacial interaction(hydrogen bonding)and mechanical entanglement endowed the nanocomposite films with excellent mechanical properties and ***,the thermal stability,water resistance,and antibacterial properties of the nanocomposite films were effectively improved with the introduction of ***,using DMAc/LiCl as the solvent system not only improves the compatibility between MCC and MXene but also avoids the problem of easy oxidation of MXene in aqueous *** the high stability of the MCC–MXene solution and enhanced properties of the MCC–MXene films,the proposed strategy manifests great potential for fabricating natural biomass-based dielectric materials.

关键词： Ti_(3)C_(2)T_(x) microcrystalline cellulose flexible dielectric thermally conductive N,N-dimethylacetamide/lithium chloride(DMAc/LiCl) compatibility

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Recent development in multizonal scaffolds for osteochondral regeneration

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Bioactive Materials 2023年第7期25卷 122-159页

作者： Le Yu Sacha Cavelier Brett Hannon Mei Wei Department of Chemical and Biomolecular Engineering Ohio UniversityAthensOH45701USA Biomedical Engineering Program Ohio UniversityAthensOH45701USA Department of Mechanical Engineering Ohio UniversityAthensOH45701USA

Osteochondral(OC)repair is an extremely challenging topic due to the complex biphasic structure and poor intrinsic regenerative capability of natural osteochondral *** contrast to the current surgical approaches which yield only short-term relief of symptoms,tissue engineering strategy has been shown more promising outcomes in treating OC defects since its emergence in the *** particular,the use of multizonal scaffolds(MZSs)that mimic the gradient transitions,from cartilage surface to the subchondral bone with either continuous or discontinuous compositions,structures,and properties of natural OC tissue,has been gaining momentum in recent *** the latest developments in the field,this review offers a comprehensive summary of recent advances,current hurdles,and future perspectives of OC repair,particularly the use of MZSs including bilayered,trilayered,multilayered,and gradient scaffolds,by bringing together onerous demands of architecture designs,material selections,manufacturing techniques as well as the choices of growth factors and cells,each of which possesses its unique challenges and opportunities.

关键词： Multizonal scaffolds Osteochondral regeneration Fabrication Cells Growth factors

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Assembly of exfoliated α-zirconium phosphate nanosheets:Mechanisms and versatile applications

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Aggregate 2022年第4期3卷 41-60页

作者： Hao Ding Abbas Ahmed Kuangyu Shen Luyi Sun Polymer Program Institute of Materials ScienceUniversity of ConnecticutStorrsConnecticutUSA Department of Chemical and Biomolecular Engineering University of ConnecticutStorrsConnecticutUSA Department of Biomedical Engineering University of ConnecticutStorrsConnecticutUSA

α-Zirconium phosphate(Zr(HPO_(4))_(2)⋅H_(2)O,α-ZrP)is an inorganic layered *** the first report of crystallineα-ZrP in 1964,thanks to its simple synthesis and unique physiochemical properties,α-ZrP has found widespread application in many fields including mechanical reinforcing,barrier improvement,flame retardancy,anticorrosion,catalysis,environment,energy,and *** of the ease of exfoliation ofα-ZrP to obtain single-layer nanosheets,as well as its rich surface chemistry thanks to the high density of orderly arranged surface acidic hydroxyl groups,α-ZrP single-layer nanosheets are ideal building blocks for self-assembly or assembly with other *** assembly ofα-ZrP nanosheets could form a randomly dispersed structure(isotropic),roughly ordered structure(nematic),or highly ordered structure(smectic)within liquid colloids or solid hybrids(including hydrogels).Thanks to the combination of the unique structures and the novel functions of the components,the assembled materials have found a wide verity of applications due to their excellent *** this article,the methods to synthesizeα-ZrP,the approaches and mechanisms to exfoliateα-ZrP,and the strategies to assembleα-ZrP nanosheets to form various structures,as well as the applications of the assembled materials are *** emerging prospects ofα-ZrP nanosheets as a key material in next-generation functional applications are envisioned.

关键词： application assembly exfoliation nanosheets α-zirconium phosphate

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Tungsten oxide-anchored Ru clusters with electron-rich and anti-corrosive microenvironments for efficient and robust seawater splitting

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SusMat 2024年第1期4卷 106-115页

作者： Yiming Zhang Weiqiong Zheng Huijuan Wu Ran Zhu Yinghan Wang Mao Wang Tian Ma Chong Cheng Zhiyuan Zeng Shuang Li College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengduChina Department of Chemical and Biomolecular Engineering National University of SingaporeSingaporeSingapore Department of Materials Science and Engineering and State Key Laboratory of Marine PollutionCity University of Hong KongKowloonHong KongChina Shenzhen Research Institute City University of Hong KongShenzhenChina

Ruthenium(Ru)has been recognized as a prospective candidate to substitute platinum catalysts in water-splitting-based hydrogen ***,minimizing the Ru contents,optimizing the water dissociation energy of Ru sites,and enhancing the long-term stability are extremely required,but still face a great ***,we report on creating tungsten oxide-anchored Ru clusters(Ru-WO_(x))with electron-rich and anti-corrosive microenvironments for efficient and robust seawater *** from the abundant oxygen vacancy structure in tungsten oxide support,the Ru-WO_(x)exhibits strong Ru-O and Ru-W bonds at the *** study elucidates that the strong Ru-O bonds in Ru-WO_(x)may accelerate the water dissociation kinetics,and the Ru-W bonds will lead to the strong metal-support interaction and electrons transfer fromWto *** optimal Ru-WO_(x)catalysts exhibit a low overpotential of 29 and 218mVat the current density of 10 mA cm^(−2) in alkaline and seawater media,*** outstanding long-term stability discloses that the Ru-WO_(x)catalysts own efficient corrosion resistance in seawater *** believe that thiswork offers new insights into the essential roles of electron-rich and anti-corrosivemicroenvironments in Ru-based catalysts and provide a new pathway to design efficient and robust cathodes for seawater splitting.

关键词： hydrogen production microenvironment modulation noble metal catalysts seawater splitting tungsten oxide

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Ultralong thermally activated delayed fluorescence based on intermolecular charge transfer induced by isomer in carbazole derivative

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Aggregate 2024年第6期5卷 392-399页

作者： Junru Chen Xianhe Zhang Zongliang Xie Bin Liu Department of Chemical and Biomolecular Engineering National University of SingaporeSingaporeSingapore Integrative Sciences and Engineering Program NUS Graduate SchoolNational University of SingaporeSingaporeSingapore Institute for Functional Intelligent Materials National University of SingaporeSingaporeSingapore

Ultralong thermally activated delayed fluorescence(UTADF)materials play an important role in realizing time-dependent color-tunable *** typical carbazole(Cz)derivatives have been reported to exhibit UTADF ***,a 10-fold difference in TADF lifetime was found between commercial Cz derivatives and the corresponding lab-synthesized ones,which indicated that UTADF may not be derived from the single Cz derivatives as *** reveal the real mechanism,we synthesized three Cz derivatives and one isomer to form three host-guest pairs for optical *** photophysical properties revealed that UTADF originated from the intermolecular charge transfer between host and guest,while the ultralong organic phosphorescence was from the *** to the rich color variations in luminescence displayed by 4-(1H-benzo[f]indol-1-yl)−4′-(9H-carbazol-9-yl)-[1,1′-biphenyl]−3,3′-dicarbonitrile/4,4′-di(9H-carbazol-9-yl)-[1,1′-biphenyl]−3,3′-dicarbonitrile(CBP-2CN)at different delay times,it can be applied to realize multi-dimensional encryption in both delay time and luminescent color.

关键词： energy transfer intermolecular charge transfer ultralong organic phosphorescence ultralong thermally activated delayed fluorescence

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