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Elucidating the promotion mechanism of the ternary cooperative heterostructure toward industrial-level urea oxidation catalysis

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Journal of Energy Chemistry 2023年第10期85卷 116-125,I0005页

作者： Xiujuan Xu Xiaotong Wei Liangliang Xu Minghua Huang Arafat Toghan School of Materials Science and Engineering Ocean University of ChinaQingdao 266100ShandongChina Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology(KAIST)291 Daehak-RoYuseong-GuDaejeon 34141Republic of Korea Chemistry Department College of ScienceImam Mohammad Ibn Saud Islamic University(IMSIU)Riyadh 11623Saudi Arabia Chemistry Department Faculty of ScienceSouth Valley UniversityQena 83523Egypt

From the perspective of electronic structure modulation,it is highly desirable to rationally design the active urea oxidation reaction(UOR)catalysts through interface *** binary cooperative heterostructure systems have been shown significant enhancement for catalyzing UOR,but their performance still remains unsatisfactory for industrialization because of the unfavorable intermediate adsorption/desorption and deficient electron transfer *** response,taking the ternary cooperative Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4) heterostructure as the proof-of-concept paradigm,a catalytic model is rationally put forward to elucidate the UOR promotion mechanism at the molecular *** rod-like Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4) nanoarrays with three-phase heterojunction are experimentally fabricated on Ni foam(named as Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4)/NF)via simple two-step *** density functional theory calculations disclose that construction of Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4) heterostructure model not only induce charge redistribution at the interfacial region for creating innumerable electron transfer channels,but also endow it with a moderate d-band center that could help to build a balance between adsorption and desorption of diverse UOR *** from the unique rod-like nanoarrays with large specific surface area and the optimized electronic structure,the well-designed Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4)/NF could act as a robust catalyst for driving UOR at industrial-level current densities under tough environments,offering great potential for commercial applications.

关键词： Urea oxidation reaction Ternary cooperative heterostructure Electronic structure Interface engineering

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Spatial Control of Lithium Deposition by Controlling the Lithiophilicity with Copper(Ⅰ)Oxide Boundaries

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Energy & Environmental Materials 2023年第5期6卷 183-191页

作者： Ju Ye Kim Oh B.Chae Gukbo Kim Woo-Bin Jung Sungho Choi Do Youb Kim San Moon Jungdon Suk Yongku Kang Mihye Wu Hee-Tae Jung Department of Chemical and Biomolecular Engineering(BK-21 four)and Institute for Nanocentury Korea Advanced Institute of Science and Technology(KAIST)DaejeonKorea Chemical&Process Technology Division Korea Research Institute of Chemical TechnologyDaejeon 34114Korea School of Engineering Brown UniversityProvidence 02912USA Department of Chemistry University of Rhode IslandKingston 02881USA School of Engineering and Applied Sciences Harvard UniversityCambridge 02138USA Advanced Materials Division Korea Research Institute of Chemical TechnologyDaejeon 34114Korea

Spatial control of lithium deposition is the most important issue in lithium-metal batteries because of the considerable control of lithium dendrite suppression via the uniform distribution of Li^(+)*** seed materials are crucial for the behavior of lithium deposition,in-depth studies on their physical and chemical control have not been ***,we describe a new design of seed structure comprising a wrinkled Cu/graphene substrate surrounded by copper(Ⅰ)oxide(Cu_(2)O)on a graphene grain boundary over a large area,which is fabricated by the oxidation of the Cu surface via graphene boundary defects by using chemical vapor deposition(CVD).Scanning and transmission electron microscopy results reveal that Cu_(2)O on the graphene boundary can render a preferential reaction with lithium during the first deposition and assist in the uniform deposition of lithium by preventing the agglomeration of lithium clusters during the second *** two-step process is attributed to the degree of selectivity due to the difference in lithium affinity,which allows long-term electrochemical stability and a high rate capability via boundary *** study highlights the significance of the boundary effect,which can open new avenues for the formation of a large family of seed structures in lithium-metal batteries.

关键词： Cu_(2)O boundary dendrite-free lithium deposition lithium-metal battery lithium spatial control seed boundary effect

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An amorphous manganese iron oxide hollow nanocube cathode for aqueous zinc ion batteries

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Journal of Energy Chemistry 2023年第12期87卷 314-321,I0008页

作者： Fengyang Jing Chade Lv Liangliang Xu Yaru Shang Jian Pei Pin Song Yuanheng Wang Gang Chen Chunshuang Yan MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HelongjiangChina Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology(KAIST)Daejeon 34141Republic of Korea Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Engineering Research Center of Carbon NeutralityCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241000AnhuiChina

Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high ***,the traditional manganese oxide cathode materials suffer from the low intrinsic electronic conductivity,sluggish ions diffusion kinetics,and structural collapse,hindering their large-scale ***,we successfully developed a latent amorphous Mn_(1.8)Fe_(1.2)O_(4) hollow nanocube(a-H-MnFeO) cathode material derived from Prussian blue analogue *** amorphous nature endows the cathode with lower diffusion barrier and narrower band gap compared with crystalline counterpart,resulting in the superior Zn^(2+) ions and electrons transport *** structure can furnish abundant surface sites and suppress the structural collapse during the repeated charge/discharge *** virtue of the multiple advantageous features,the a-H-MnFeO cathode exhibits exceptional electrochemical performance,in terms of high capacity,excellent rate capability,and prolonged cycle *** strategy will pave the way for the structural design of emerging cathode materials.

关键词： Aqueous zinc-ion batteries Manganese iron oxide cathode Amorphous structure Hollow nanostructure lons transport kinetics

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A Stretchable Glucose Sensor via Conductive Polymer-Coated VACNT Forests Rooted in Elastomer Polymer Substrate

IEEE Journal on Flexible Electronics

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IEEE Journal on Flexible Electronics 2023年第3期2卷 274-281页

作者： Palumbo, Anthony Wang, Hongjun Levon, Kalle Yang, Eui-Hyeok Stevens Institute of Technology Department of Mechanical Engineering HobokenNJ07030 United States Stevens Institute of Technology Department of Biomedical Engineering HobokenNJ07030 United States New York University Chemical and Biomolecular Engineering Tandon School of Engineering BrooklynNY11201 United States Stevens Institute of Technology Department of Mechanical Engineering and the Center for Quantum Science and Engineering HobokenNJ07030 United States

This article presents a stretchable glucose sensor composed of dodecylbenzenesulfonate-doped polypyrrole (PPyDBS)-coated vertically aligned carbon nanotube (VACNT) forests rooted in polydimethylsiloxane (PDMS) substrate. The measured sensitivity was approximately 10 mAcm-2M-1 with a wide linear range demonstrated, as low as 0.1 mM and up to 12 mM, and the sensor achieved 90% of steady-state current in less than 3 s. The PDMS/CNT/PPy(DBS)/GOx structure was tested under stretching, demonstrating the coefficients of determination larger than 0.982, indicating its robustness of sensing capability of glucose concentrations with tensile strain up to 75%. These results show the potential of this stretchable glucose sensor with a novel fabrication strategy and stretchable electrode design toward potential wearable applications interfacing with physiological fluids. © 2022 IEEE.

关键词： Glucose

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Transport cocktails for cancer therapeutics

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Physical Review Research 2024年第3期6卷 033137-033137页

作者： Michail E. Kavousanakis Omkar Bhatavdekar Remco Bastiaannet Yannis Kevrekidis Stavroula Sofou School of Chemical Engineering Department of Chemical and Biomolecular Engineering Institute for NanoBioTechnology Department of Radiology and Radiological Science School of Medicine

Beyond biological cell heterogeneity, evidenced by different resistances to therapeutics, “delivery heterogeneity” crucially limits treatment efficacy for advanced solid tumors: variations in therapeutic drug delivery to different tumor areas (perivascular, perinecrotic) leading to nonuniform drug concentrations/doses and to unsuccessful treatment (cancer cell kill). Short-range (40–80 µm), high energy (1–5 MeV) α particles successfully address the biological heterogeneity: the double-strand DNA breaks they cause make them impervious to cell resistance mechanisms. Multiresponsive nanocarriers and/or engineered antibody-drug-conjugates are elegant approaches to delivering such α-particle emitters. Delivery heterogeneity, however, remains a challenge in established (i.e., large, vascularized) tumors. Remarkably, delivery properties enabling efficacy at the cell scale (targeting selectivity, affinity, cell drug uptake) may act against spatial delivery uniformity at the tumor scale (binding-site barrier effect). We have previously demonstrated, in different mouse models, that spatial delivery uniformity, key to the effective killing of solid tumors, can be achieved utilizing combinations of different, distinct delivery carriers of the same emitter, but with different, complementary delivery properties, “leaving no cancer cell behind.” We build first principles reaction-transport models (quantitatively informed by experiments) that explain the “geographically complementary” behaviors of such carrier cocktails, and help optimally design these cocktails and their delivery protocols.

关键词： Cancer Drug delivery Radiation therapy

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Effect of exogenous flavins on the microbial corrosion by Geobacter sulfurreducens via iron-to-microbe electron transfer

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Journal of Materials science & Technology 2024年第4期171卷 129-138页

作者： Yuting Jin Jiaqi Li Mingxing Zhang Borui Zheng Dake Xu Tingyue Gu Fuhui Wang Shenyang National Laboratory for Materials Science Northeastern UniversityShenyang 110819China Key Laboratory for Anisotropy and Texture of Materials(Ministry of Education) Northeastern UniversityShenyang 110819China Department of Chemical and Biomolecular Engineering Institute for Corrosion and Multiphase TechnologyOhio UniversityAthens OH 45701USA

Microbes can cause or accelerate metal corrosion,leading to huge losses in corrosion damages each *** sulfurreducens is a representative electroactive bacterium in many soils,sediments,and wastew-ater *** has been confirmed to directly extract electrons from elemental ***,little is known about the effect of electron shuttles in *** corrosion on stainless *** this study,we report that exogenous flavins promote iron-to-microbe electron transfer,accelerating micro-bial *** caused 1.3 times deeper pits and increased electron uptake(with 2 times increase of i_(corr))from stainless steel when riboflavin was added to the culture ***-deficient mutant data suggest that *** utilizes riboflavin as a bound-cofactor in outer membrane c-type *** finding that,in the presence of microbes,riboflavin can substantially accelerate corrosion highlights the role of flavin redox cycling for enhanced iron-to-microbe electron transfer by *** and provides new insights in microbial corrosion.

关键词： Extracellular electron transfer Microbiological corrosion Geobacter sulfurreducens Outer membrane c-type cytochromes Exogenous flavins

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Electrically conductive nanowires controlled one pivotal route in energy harvest and microbial corrosion via direct metal-microbe electron transfer

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Journal of Materials science & Technology 2024年第7期174卷 226-233页

作者： Yuting Jin Jiaqi Li Toshiyuki Ueki Borui Zheng Yongqiang Fan Chuntian Yang Zhong Li Di Wang Dake Xu Tingyue Gu Fuhui Wang Shenyang National Laboratory for Materials Science Northeastern UniversityShenyang 110819China Key Laboratory for Anisotropy and Texture of Materials(Ministry of Education) Northeastern UniversityShenyang 110819China Department of Chemical and Biomolecular Engineering Institute for Corrosion and Multiphase TechnologyOhio UniversityAthensOH 45701USA

Extracellular electron transfer(EET)plays a critical role in bioelectrochemical processes,allowing cou-pling between microorganisms and extracellular solid-state electrodes,metals,or other cells in energy *** studies have suggested a role for outer-surface c-type cytochromes in direct metal-to-microbe electron transfer by Geobacter sulfurreducens,a model electroactive ***,we ex-amined the possibility of other microbially produced electrical contacts by deleting the gene for PilA,the protein monomer that *** assembles into electrically conductive protein nanowires(e-pili).Deleting pilA gene inhibited electron extraction from pure iron and 316L stainless steel up to 31%and 81%,respectively more than deleting the gene for the outer-surface cytochrome *** PilA-deficient phenotype,and the observation that relatively thick biofilms(21.7μm)grew on the metal surfaces at multi-cell distances from the metal surfaces suggest that e-pili contributed significantly to microbial cor-rosion via direct metal-to-microbe electron *** results have implications for the fundamental understanding of electron harvest via e-pili by electroactive microbes,their uses in bioenergy production,as well as in monitoring and mitigation of metal biocorrosion.

关键词： Electrically conductive protein nanowires Direct metal-to-microbe electron transfer Geobacter sulfurreducens Outer-surface c-type cytochromes Biofilm

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Application of a Self-Assembly Sensing Layer to Grating Sensor Cabinets for Biomedical Sensing of Rheumatoid Arthritis Antigen-Antibodies

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IEEE Sensors Journal 2024年第7期24卷 10039-10047页

作者： Wen, Hsin-Yi Hsu, Hsiang-Cheng Feng, Wen-Kai Jhan, Kai-Siang Yeh, Yao-Tsung Chiang, Chia-Chin National Kaohsiung University of Science and Technology Department of Chemical and Materials Engineering Kaohsiung80778 Taiwan National Kaohsiung University of Science and Technology College of Maritime Department of Ph.D. Program in Maritime Science and Technology Kaohsiung807618 Taiwan National Kaohsiung University of Science and Technology Department of Mechanical Engineering Kaohsiung80778 Taiwan Fooyin University Department of Medical Laboratory Science and Biotechnology Kaohsiung83102 Taiwan

In this article, we harnessed biomedical applications in laser-assisted etching long-period fiber gratings (LLPFGs) sensors, subsequently deploying them within the realm of biomedical applications. The primary aim of this study was to devise a sensitive method for the detection of antigen-antibodies associated with rheumatoid arthritis (RA) using LLPFGs. Sensing the antigen binding took place on the surface of the optical fiber through a self-assembling process. Given the inherent limitations of conventional rheumatoid factor (RF) testing in terms of specificity, we introduced an innovative serum-based approach geared toward the identification of anti-cyclic citrullinated peptide (Anti-CCP) antibodies. This method exhibited an impressive diagnostic accuracy rate of approximately 80% for RA cases, coupled with an exceptional specificity level of 98% for individuals without RA. The incorporation of LLPFGs in the detection of RA antigen-antibodies presents a highly promising avenue for enhancing the precision and reliability of RA diagnosis. Furthermore, this research aligns closely with the United Nations Sustainable Development Goal (SDG)3, which strives to promote well-being across all age groups and advance sustainable development by addressing health-related challenges, including the accurate diagnosis of diseases like RA. © 2023 IEEE.

关键词： Antibodies

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A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li-S Batteries (vol 9, pg 3869, 2024)

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ACS ENERGY LETTERS 2024年第9期9卷 4524-4525页

作者： Qin, Kaiqiang Li, Shi Yen, Dean Zhang, Weiran Yang, Zhenzhen Kamphaus, Ethan Phillip Kim, Eric Youngsam Huang, Jinghao Shea, John J. Hu, Enyuan Cheng, Lei Wang, Chunsheng Luo, Chao Department of Chemistry and Biochemistry George Mason University Fairfax Virginia 22030 United States Materials Science Division Argonne National Laboratory Lemont Illinois 60439 United States Chemistry Division Brookhaven National Laboratory Upton New York 11973 United States Department of Chemical and Biomolecular Engineering University of Maryland College Park Maryland 20742 United States Chemical Sciences and Engineering Division Argonne National Laboratory Lemont Illinois 60439 United States Department of Chemical Environmental and Materials Engineering University of Miami Coral Gables Florida 33146 United States Chemical Sciences Division Oak Ridge National Laboratory Oak Ridge Tennessee 37831 United States Quantum Science & Engineering Center George Mason University Fairfax Virginia 22030 United States

The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte conditions. Herein, a LiF-rich SEI and a LiF–LixNyOzcoenriched CEI are simultaneously formed by adding ionic liquid (Py13TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. The LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN, therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm–2) pouch cells under the lean electrolyte conditions (E/S ratio of 5 mL gSPAN–1) deliver a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium–sulfur batteries.

关键词： Cathodes

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Inhibiting scar formation via wearable multilayer stacked electret patch:Self-creation of persistent and customizable DC electric field for fibrogenic activity restriction

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InfoMat 2024年第3期6卷 66-80页

作者： Sung-Won Kim Sumin Cho Donghan Lee Jiyu Hyun Sunmin Jang Inwoo Seo Hyun Su Park Hee Jae Hwang Hyung-Seop Han Dae Hyeok Yang Heung Jae Chun Suk Ho Bhang Dongwhi Choi School of Chemical Engineering Sungkyunkwan UniversitySuwonRepublic of Korea Department of Mechanical Engineering(Integrated Engineering Program) Kyung Hee UniversityYonginGyeonggiRepublic of Korea Biomaterials Research Center Biomedical Research DivisionKorea Institute of Science and Technology(KIST)SeoulRepublic of Korea Department of Medical Life Sciences College of MedicineInstitute of Cell and Tissue EngineeringThe Catholic University of KoreaSeoulRepublic of Korea

Electrical stimulation has recently received attention as noninvasive treatment in skin wound healing with its outstanding biological property for clinical ***,the complexity of equipment for applying appropriate electrical stimulation remains an ongoing ***,we proposed a strategy for skin scar inhibition by providing electrical stimulation via a multilayer stacked electret(MS-electret),which can generate direct current(DC)electric field(EF)without any power supply *** addition,the MS-electret can easily control the intensity of EFs by simply stacking electret layers and maintain stable EF with the surface potential of 3400 V over 5 days owing to the injected charges on the electret *** confirmed inhibition of type 1 collagen andα-SMA expression of human dermal fibroblasts(hDFs)by 90%and 44%in vitro,indicating that the transition of hDFs to myofibroblasts was restricted by applying stable electrical *** further revealed a 20%significant decrease in the ratio of myofibroblasts caused by the MS-electret in *** findings present that the MS-electret is an outstanding candidate for effective skin scar inhibition with a battery-free,physiological electrical microenvironment,and noninvasive treatment that allows it to prevent external infection.

关键词： DC electric field dermal fibroblasts electret scar formation restriction self-creation of electrical stimulation

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