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ACS Electrochemistry 2024年第3期1卷 328-337页

作者： Yousef A. Alsunni Abdulaziz W. Alherz Charles B. Musgrave Chemical Engineering Department King Fahd University of Petroleum and Minerals Dhahran 31261 Saudi Arabia；Department of Chemical and Biological Engineering University of Colorado Boulder Colorado 80309 United States Department of Chemical Engineering College of Engineering and Petroleum Kuwait University Safat 13060 Kuwait Department of Chemical and Biological Engineering University of Colorado Boulder Colorado 80309 United States；Renewable and Sustainable Energy Institute University of Colorado Boulder Colorado 80309 United States；Materials Science and Engineering Program University of Colorado Boulder Colorado 80309 United States

Grand canonical density functional theory (GC-DFT) was employed to model the electrocatalytic reduction of CO2(CO2R) to CO by single titanium atom nitrogen-doped graphene, referred to as Ti@4N-Gr. Previous GC-DFT thermodynamic investigations have identified Ti@4N-Gr as a promising CO2R catalyst; however, no in-depth studies have examined it. In this study, we analyze activation energies of the elementary steps at various applied potentials in addition to thermodynamics of CO2R to CO catalyzed by Ti@xN-Gr defects. Reaction intermediates are predicted to be destabilized when Ti is coordinated to fewer N atoms. Based on reaction thermodynamics, Ti@4N-Gr and all defect configurations are predicted to be potentially promising catalysts for CO2R to CO at an applied potential of −0.7 VSHEwhile at −0.3 and −1.2 VSHEthe reaction is predicted to be hindered by relatively large grand free energy differences between intermediates. We propose a criterion to identify optimum applied potentials for CO2R to CO based on the potential of zero charge (PZC) of the reaction intermediates and the contention that the optimum applied potential for CO2R to CO lies in the rangePZC*CO

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ROS-sensitive PD-L1 siRNA cationic selenide nanogels for self-inhibition of autophagy and prevention of immune escape

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Bioactive Materials 2024年第11期41卷 597-610页

作者： Jie Gao Yonghua Zhai Weihong Lu Xianghe Jiang Jingsheng Zhou Lili Wu Longhai Du Chunqing Ou Xinyi Zhang Hanliang He Jian Zhu Zhengbiao Zhang Meiyun Li Yan Wu Xiangqiang Pan State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China Changhai Clinical Research Unit Shanghai Changhai HospitalNaval Medical UniversityShanghai200433China Shanghai Key Laboratory of Nautical Medicine and Translation of Drugs and Medical Devices Shanghai200433China College of Life Science Mudanjiang Medical UniversityMudanjiang157011China Department of Orthopedics Jinshan HospitalFudan UniversityShanghai201508China The Department of Orthopedic Surgery Dushu Lake Hospital Affiliated to Soochow UniversitySuzhou215028China

In the field of cancer therapy,inhibiting autophagy has emerged as a promising ***,pharmacological disruption of autophagy can lead to the upregulation of programmed death-ligand 1(PD-L1),enabling tumor immune *** address this issue,we developed innovative ROS-responsive cationic poly(ethylene imine)(PEI)nanogels using selenol chemistry-mediated multicomponent reaction(MCR)*** procedure involved simple mixing of low-molecular-weight PEI(LMW PEI),γ-selenobutylacetone(γ-SBL),and poly(ethylene glycol)methacrylate(PEGMA).Through high-throughput screening,we constructed a library of AxSeyOz nanogels and identified the optimized A1.8Se3O0.5/siPD-L1 nanogels,which exhibited a size of approximately 200 nm,excellent colloidal stability,and the most effective PD-L1 silencing *** nanogels demonstrated enhanced uptake by tumor cells,excellent oxidative degradation ability,and inhibited autophagy by alkalinizing *** A1.8Se3O0.5/siPD-L1 nanogels significantly downregulated PD-L1 expression and increased the expression of major histocompatibility complex class I(MHC-I),resulting in robust proliferation of specific CD8+T cells and a decrease in MC38 tumor *** a result,the A1.8Se3O0.5/siPD-L1 nanogels inhibited tumor growth through self-inhibition of autophagy,upregulation of MHC-I,and downregulation of *** with dynamic diselenide bonds,the A1.8Se3O0.5/siPD-L1 nanogels showed synergistic antitumor efficacy through self-inhibition of autophagy and prevention of immune escape.

关键词： Multicomponent reaction ROS sensitive Cationic nanogel Autophagy inhibition Immune escape

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Regulating the Electron Localization of Metallic Bismuth for Boosting CO_(2)Electroreduction

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Nano-Micro Letters 2022年第2期14卷 296-310页

作者： Dan Wu Renfei Feng Chenyu Xu Peng-Fei Sui Jiujun Zhang Xian-Zhu Fu Jing-Li Luo Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China Canadian Light Source Inc. SaskatoonSaskatchewan S7N 0X4Canada Department of Chemical and Materials Engineering University of AlbertaEdmontonAB T6G 1H9Canada Institute for Sustainable Energy/College of Science Shanghai UniversityShanghai 200444People’s Republic of China

Electrochemical reduction of CO_(2)to formate is economically attractive but improving the reaction selectivity and activity remains ***,we introduce boron(B)atoms to modify the local electronic structure of bismuth with positive valence sites for boosting conversion of CO_(2)into formate with high activity and selectivity in a wide potential *** combining experimental and computational investigations,our study indicates that B dopant differentiates the proton participations of rate-determining steps in CO_(2)reduction and in the competing hydrogen *** comparing the experimental observations with the density functional theory,the dominant mechanistic pathway of B promoted formate generation and the B concentration modulated effects on the catalytic property of Bi are *** comprehensive study offers deep mechanistic insights into the reaction pathway at an atomic and molecular level and provides an effective strategy for the rational design of highly active and selective electrocatalysts for efficient CO_(2)conversion.

关键词： CO_(2)reduction Bismuth Proton transport Electron localization Boron

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Three-dimensional oscillation of an acoustic microbubble between two rigid curved plates

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Journal of Hydrodynamics 2021年第5期33卷 1019-1034页

作者： Kawa M.A.Manmi Imad A.Aziz Arun Arjunan Rostam K.Saeed Abdolrahman Dadvand Department ofMathematics College of ScienceSalahaddin University-ErbilKurdistan RegionIraq Department of Information Technology College of Engineering and Computer ScienceLebanese French UniversityKurdistan RegionIraq Faculty of Science and Engineering University of WolverhamptonWolverhamptonUK Faculty of Mechanical Engineering Urmia University of TechnologyUrmiaIran Karlsruhe Institute of Technology(KIT) Institute for Chemical Technology and Polymer ChemistryKarlsruheGermany

Understanding the near boundary acoustic oscillation of microbubbles is critical for the effective design of ultrasonic biomedical devices and surface cleaning ***,this study investigates the three-dimensional microbubble oscillation between two curved rigid plates experiencing a planar acoustic field using boundary integral method(BIM).The numerical model is validated via comparison with the nonlinear oscillation of the bubble governed by the modified Rayleigh-Plesset equation and with the axisymmetric model for an acoustic microbubble in infinite fluid ***,the influence of the wave direction and horizontal standoff distance(h)on the bubble dynamics(including jet velocity,jet direction,centroid movement,total energy,and Kelvin impulse)were *** was concluded that the jet velocity,the maximum radius and the total energy of the bubble are not significantly influenced by the wave direction,while the jet direction and the high-pressure region depend strongly on *** importantly,it was found that the jet velocity and the high-pressure region around the jet in acoustic bubble are drastically larger than their counterparts in the gas bubble.

关键词： Acoustic microbubble bubble dynamics boundary integral method(BIM) two curved plates potential flow

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Gap engineering of sandwich plasmonic gap nanostructures for boosting plasmon-enhanced electrocatalysis

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Nano Research 2023年第7期16卷 8961-8969页

作者： Lu Cheng Fengxia Wu Yu Tian Xiali Lv Fenghua Li Guobao Xu Hsien-Yi Hsu Yongjun Zhang Wenxin Niu State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Yanshan Branch of Beijing Chemical Research Institute SinopecBeijing 102500China University of Science and Technology of China Hefei 230026Chin a 4 School of Energy and Environment Department of Materials Science and EngineeringCity University of Hong KongKowloon TongHong Kong 999077China Shenzhen Research Institute of City University of Hong Kong Shenzhen 518057China Key Laboratory of Functional Polymer Materials and State Key Laboratory of Medicinal Chemical Biology Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

Plasmonic catalysis is emerging as a dynamic field in heterogeneous catalysis and holds great promise for the efficient utilization of solar *** to the development of plasmonic catalysis is the design of efficient plasmonic *** this report,plasmonic gap nanostructures(PGNs)on the basis of Au@poly(o-phenylenediamine)(POPD)@Pd sandwich nanostructures are synthesized as plasmonic nanocatalysts by an in-situ reduction synthetic strategy,which allows for the precise engineering of the POPD gap size between plasmonic Au and catalytic Pd *** introduction of conducting POPD nanogap in PGNs not only effectively enhances their light harvesting capability,but also provides an effective charge transfer channel for harnessing the photogenerated hot charge *** this respect,distinct gap-dependent performances in plasmon-enhanced electrocatalysis of ethanol oxidation reactions(EOR)are demonstrated with the PGN nanocatalysts and over 2.5 folds of enhancement can be achieved.A volcano plot is derived to describe the relationship between the catalytic activities and gap size of the PGN nanocatalysts,which is well explained by the interplay of their light harvesting and charge transport *** results highlight the importance of gap engineering in PGNs for plasmonic catalysis and offer the promise of developing efficient plasmonic nanocatalysts for other heterogeneous catalytic reactions.

关键词： plasmonic gap nanostructures electrocatalysis ethanol oxidation reactions light harvesting charge transport

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Impact of alloy-like phase on energy loss mitigation in multi-component organic photovoltaics

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Aggregate 2024年第4期5卷 339-348页

作者： Xiangyue Kong Lingling Zhan Zhongjie Li Yaxin Yang Yuhao Liu Huayu Qiu Xiaokang Sun Hanlin Hu Rui Sun Jie Min Shouchun Yin Weifei Fu Hongzheng Chen Key Laboratory of Organosilicon Chemistry and Materials Technology of Ministry of Education College of MaterialsChemistry and Chemical EngineeringHangzhou Normal UniversityHangzhouP.R.China Hoffmann Institute of Advanced Materials Shenzhen Polytechnic UniversityShenzhenP.R.China The Institute for Advanced Studies Wuhan UniversityWuhanP.R.China State Key Laboratory of Silicon and Advanced Semiconductor Materials Department of Polymer Science and EngineeringZhejiang UniversityHangzhouP.R.China

The multi-component strategy has proven effective in advancing the performance of organic photovoltaics(OPVs),enhancing photocurrent andfill factor through spectral complementarity and morphology ***,the open-circuit voltage(VOC)mechanism in multi-component systems lacks systematic *** this study,we explore the influence of alloy-like phases on energy level distribution and energy loss mechanisms in multi-component *** modulation of donor alloy-like phases maintains the original intermolecular stack-ing,enhances component compatibility,reduces acceptor aggregation,and improves acceptor phase purity,mitigating non-radiative recombination ***,suitable alloy-like phase modulation elevates charge transfer(CT)states,reducing the gap between CT and local exciton state,lowering reorganization energy,and alleviating radiative recombination loss below the *** synergistic optimization(layer-by-layer method with solid additive),ternary devices based on Y6 acceptor achieve a notable 19.41%power conversion efficiency,offering new insights for the analysis of the energy loss of the multi-component OPVs.

关键词： alloy-like phase charge transfer state energy loss high efficiencies multi-donors

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2D-Transition Metal Borides (MBenes): a comprehensive review of the materials, chemistry, advances, and novel applications

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Advanced Composites and Hybrid Materials 2025年第3期8卷 1-50页

作者： Ramezanzadeh, Mohammad Ghamarpoor, Reza Dashan, Ali Fallah, Akram Soleimani, Soolmaz Ramezanzadeh, Bahram Iran Polymer and Petrochemical Institute Tehran Iran Department of Petroleum Engineering Faculty of Engineering University of Garmsar Garmsar Iran Department of Surface Coatings and Corrosion Institute for Color Science and Technology Tehran Iran Department of Chemical Technologies Iranian Research Organization for Science and Technology (IROST) Tehran Iran Department of Marine Paint Pars Pamchal Chemical Co. Qazvin Iran

MBenes and MAB phases are emerging classes of materials with unique properties and potential applications. MAB phases, first introduced in 2017, are ternary compounds with a layered structure similar to MAX phases but with boron replacing carbon. These materials have attracted significant attention due to their outstanding mechanical, electrical, and structural properties. MBene phases, derived from MAB phases through selective etching, are 2D materials analogous to MXenes, exhibiting high conductivity, chemical stability, and a broad range of applications. This review provides an in-depth analysis of MBene and MAB phases, including their structures, properties, synthesis methods, and applications. The history of MAB phase discovery and its evolution into MBene phases is discussed, along with advancements in synthesis techniques and the challenges associated with their production. The review also covers characterization methods for these materials, highlighting their distinct features. The properties of MBenes and MAB phases are explored, with a focus on their applications in energy storage, including supercapacitors and batteries, and their catalytic performance in reactions such as the Hydrogen Evolution Reaction (HER), Nitrogen Reduction Reaction (NRR), Carbon Dioxide Reduction Reaction (CO2RR), Oxygen Reduction Reaction (ORR), Nitric Oxide Reduction Reaction (NORR), and Carbon Capture and Storage (CCS). Additionally, their potential in biological and photocatalytic applications is discussed. Lastly, this review addresses the challenges associated with the synthesis and utilization of MBenes and MAB phases. By providing a comprehensive overview from their discovery to their current applications and limitations, this article aims to serve as a foundational resource for researchers and practitioners in the field.

关键词： MAB phases MBenes Transition metal borides (TMB) MXenes

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Amination of biochar surface from watermelon peel for toxic chromium removal enhancement

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Chinese Journal of chemical engineering 2021年第8期34卷 199-222页

作者： Mohamed A.El-Nemr Ibrahim M.A.Ismail Nabil M.Abdelmonem Ahmed El Nemr Safaa Ragab Department of Chemical Engineering Faculty of EngineeringCairo UniversityGizaEgypt Renewable Energy Program Zewail City of Science and TechnologyEgypt Environmental Division National Institute of Oceanography and FisheriesKayet BeyEl-AnfoushyAlexandriaEgypt

Watermelon peel residues were used to produce a new biochar by dehydration *** new biochar has undergone two methods of chemical modification and the effect of this chemical modification on its ability to adsorb Cr(VI)ions from aqueous solution has been *** biochars,Melon-B,Melon-BO-NH_(2) and Melon-BO-TETA,were made from watermelon peel via dehydration with 50%sulfuric acid to give Melon-B followed by oxidation with ozone and amination using ammonium hydroxide to give Melon-BO-NH_(2) or Triethylenetetramine(TETA)to give *** prepared biochars were characterized by BET,BJH,SEM,FT-IR,TGA,DSC and EDAX *** highest removal percentage of Cr(VI)ions was 69%for Melon-B,98%for Melon-BO-NH_(2) and 99%for Melon-BO-TETA biochars of 100 mg·L^(−1) Cr(VI)ions initial concentration and 1.0 g·L^(−1) adsorbents *** unmodified biochar(Melon-B)and modified biochars(Melon-BO-NH_(2) and Melon-BO-TETA)had maximum adsorption capacities(Q_(m))of 72.46,123.46,and 333.33 mg·g^(−1),*** amination of biochar reduced the pore size of modified biochar,whereas the surface area was *** obtained data of isotherm models were tested using different error function *** Freundlich,Tempkin and Langmuir isotherm models were best fitted to the experimental data of Melon-B,Melon-BO-NH_(2) and Melon-BO-TETA,*** adsorption rate was primarily controlled by pseudo-second–order rate ***,the functional groups interactions are important for adsorption mechanisms and expected to control the adsorption *** adsorption for the Melon-B,Melon-BO-NH_(2) and Melon-BO-TETA could be explained for acid–base interaction and hydrogen bonding interaction.

关键词： Waste treatment Powder technology Citrullus lanatus Hexavalent chromium Biochar amination Adsorption

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Ni-based bimetallic surface alloy catalysts for enhanced poisoning resistance in steam methane reforming: A combined DFT and experimental study

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International Journal of Hydrogen Energy 2025年 144卷 152-164页

作者： Cha, Hwa-Woong Song, Giseong Min, Kyeongseok Akpe, Shedrack G. Kim, Junseong Yoon, Sung Pil Baeck, Sung-Hyeon Ham, Hyung Chul Department of Chemistry and Chemical Engineering Education and Research Center for Smart Energy and Materials Inha University Incheon22212 Korea Republic of Program in Energy Process Innovation Convergence Inha University Incheon22212 Korea Republic of Center for Hydrogen Fuel Cell Research Korea Institute of Science and Technology 5 Hwarang-ro 14-gil Seongbuk-gu Seoul02792 Korea Republic of

This study investigates the activities of Ni-M (M = transition metals) bimetallic catalysts in Molten Carbonate Electrolysis Cells (MCEC) for hydrogen production via steam methane reforming (SMR) under electrolyte poisoning conditions by using the density functional theory (DFT) and experimental approach. Focusing on the cost-effective and high-activity Ni (211) catalyst, the study addresses the challenge of electrolyte (Li2CO3, K2CO3) evaporation leading to catalyst deactivation. Utilizing DFT, we examined partially electrolyte-poisoned Ni (211) slab models, particularly assessing potassium (K) atom effects. The study proposes bimetallic Ni-M surface alloy catalysts, such as Ni–V, demonstrating enhanced electrolyte poisoning resistance and superior catalytic activity compared to pure Ni. The findings highlight the potential of these catalysts to improve MCEC system efficiency, offering a more economical alternative to precious metal catalysts. © 2025 Hydrogen Energy Publications LLC

关键词： Steam reforming

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Leveraging Non-Covalent Interactions to Control the Morphology and Electrical and Mechanical Properties of Stretchable Semiconducting Composites

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Chemistry of Materials 2023年第22期35卷 9713-9724页

作者： Wang, Yunfei Chen, Kai-Lin Awada, Angela Prine, Nathaniel Cao, Zhiqiang Zhu, Chenhui Chiu, Yu-Cheng Rondeau-Gagné, Simon Gu, Xiaodan School of Polymer Science and Engineering Center for Optoelectronic Materials and Devices The University of Southern Mississippi HattiesburgMS39406 United States Department of Chemical Engineering National Taiwan University of Science and Technology Taipei106 Taiwan Department of Chemistry and Biochemistry Advanced Materials Centre of Research University of Windsor WindsorONN9B3P4 Canada Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States

Physical blending conjugated polymers (CPs) with elastomers has been established as an effective method for enhancing the stretchability of semiconductors. However, predictable control of the morphology for incompatible polymer rubber blends remains a challenge. In this work, we demonstrated the control of phase separation size of CP/elastomer composites by strategically controlling the location sites of H-bonding functional groups in CPs and elastomers, while investigating their effects on mechanical and electrical properties. We incorporated amide functional groups into a DPP-based semiconducting polymer (DPPTVT-A) and polyisobutylene-based elastomer (PIB-A) to enable inter- and intraphase hydrogen bonding (H-bonding) cross-links within CP/elastomer composites. Along with their nonamide counterparts, we fabricated four different CP/elastomer composites, DPPTVT-A/PIB-A, DPPTVT-A/PIB, DPPTVT/PIB-A, and DPPTVT/PIB, with dual-, uni-, and non-H-bonding cross-links and compared their phase behavior and electronic and mechanical properties. The location of the H-bonding greatly influenced the property of the semiconducting rubber as characterized by scattering, spectroscopy, and electrical characterization. Importantly, we found that creating a H-bonding cross-link into both domains of CP/elastomer composites can not only improve energy dissipation upon stretching but also maintain the electrical performance when applying high tensile stress. This work provides a comprehensive study of the morphology of CP/elastomer composites, offering valuable insights into the future design of stretchable CP/elastomer composites. © 2023 American chemical Society

关键词： Hydrogen bonds

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