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Direct synthesis of large-area Al-doped graphene by chemical vapor deposition:Advancing the substitutionally doped graphene family

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Nano Research 2022年第2期15卷 1310-1318页

作者： Sami Ullah Yu Liu Maria Hasan Wenwen Zeng Qitao Shi Xiaoqin Yang Lei Fu Huy Q.Ta Xueyu Lian Jingyu Sun Ruizhi Yang Lijun Liu Mark H.Rummeli College of Energy Soochow Institute for Energy and Materials Innovations Soochow UniversitySuzhou 215006China Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China NUTECH School of Applied Sciences&Humanities and Computer Engineering Department National University of TechnologyIslamabad 42000Pakistan Centre of Polymer and Carbon Materials Polish Academy of SciencesM.Curie-Sklodowskiej 34Zabrze 41-819Poland School of Energy and Power Engineering Xian Jiaotong UniversityXian 710049China College of Chemistry and Molecular Science Wuhan UniversityWuhan 430072China Institute for Complex Materials IFW Dresden 20 Helmholtz Strasse Dresden 01069Germany Institute of Environmental Technology VSB-Technical University of Ostrava17.listopadu 15Ostrava 70833Czech Republic

Graphene doping continues to gather momentum because it enables graphene properties to be tuned,thereby affording new properties to,improve the performance of,and expand the application potential of *** can be chemically doped using various methods such as surface functionalization,hybrid composites(e.g.,nanoparticle decoration),and substitution doping,wherein C atoms are replaced by foreign ones in the graphene *** works have predicted that graphene could be substitutionally doped by aluminum(Al)atoms,which could hold promise for exciting applications,including hydrogen storage and evolution,and *** theoretical predictions suggest that Al substitutionally doped graphene(AIG)could serve as a material for gas sensors and the catalytic decomposition of undesirable ***,fabricating Al substitutionally doped graphene has proven challenging until ***,we demonstrate how controlled-flow chemical vapor deposition(CVD)implementing a simple solid precursor can yield high-quality and large-area monolayer AIG,and this synthesis is unequivocally confirmed using various characterization methods including local electron energy-loss spectroscopy(EELS).Detailed high-resolution transmission electron microscopy(HRTEM)shows numerous bonding configurations between the Al atoms and the graphene lattice,some of which are not theoretically ***,the produced AIG shows a CO_(2) capturability superior to those of other substitutionally doped graphenes.

关键词： aluminum-doped graphene single-solid precursor chemical vapor deposition carbon dioxide capture energy storage catalytic applications

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Surface Pegylation of Pan Membrane Via Cationic Photopolymerization for Enhanced Antifouling, Hemocompatibility and Separation Performance

SSRN

引用

SSRN 2023年

作者： Wen, Shaobin Wang, Yan Zhang, Jingyu Fan, Liyuan Zhang, Qiang Deng, Yufei Xin, Yangyang Zou, Yingquan Key Laboratory of New Membrane Materials Ministry of Industry and Information Technology School of Environmental and Biological Engineering Nanjing University of Science and Technology Nanjing210094 China Institute of Polymer Ecomaterials School of Environmental and Biological Engineering Nanjing University of Science and Technology Nanjing210094 China Hubei Gurun Technology Co. Ltd. Jingmen448000 China Department of Applied Chemistry College of Chemistry Beijing Normal University Beijing100875 China

Poly(acrylonitrile) (PAN) is one of the most widely-used membrane materials. However, its low hydrophilicity and biocompatibility lead to relatively poor anti-fouling and hemocompatibility of membrane. Herein, surface PEGylation of PAN membrane is conducted to enhance its antifouling, hemocompatibility and separation performance. Rapid cationic photopolymerization of poly (ethylene glycol) (PEG) with terminal oxetane groups could generate a cross-linked PEG network on the membrane surface. The structure and separation performance of membrane could be regulated by adjusting the molecular weight of PEG and the UV radiation time. The hydrophilicity of membrane has been significantly enhanced due to the PEGylation. Compared with pristine PAN membrane, the adsorption of BSA on PAN/PEG 200 decreased from 42.3 μg cm−2 to 13.38 μg cm−2 and it had higher flux recovery after filtering the BSA solution. The hemocompatibility of PEGylated membrane also improved, including anti-adsorption to platelet and erythrocyte, low hemolysis rate (~1%) and prolonged plasma coagulation time (~11.8 min). PEGylated membrane also showed excellent fractionation performance to dye/salt with the rejection of 98.4% to CBB and only 8.0% to NaCl. The membrane has shown superior chlorine resistance, with flux and retention remaining stable over a 14-day test. The PEGylation by cationic photopolymerization in this research is fast and facile, which may have potential application in the fabrication of antifouling and biocompatible membranes. © 2023, The Authors. All rights reserved.

关键词： Membranes

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Novel Biopromoter for Gas Hydrate Formation: Application to Solidified Methane Storage

SSRN

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SSRN 2023年

作者： Seo, Yongwon Farhadian, Abdolreza Mohammadi, Abolfazl Maddah, Mina Sadeh, Elaheh Nowruzi, Reza Sharifi, Ruhollah Rizi, Zahra Taheri Taheri, Mahbobeh Mohammad Department of Petroleum Engineering Kazan Federal University Kremlevskaya str. 18 Kazan420008 Russia Department of Polymer & Materials Chemistry Faculty of Chemistry and Petroleum Science Shahid Beheshti University GC Tehran*** Iran Department of Chemical Engineering University of Bojnord Bojnord*** Iran School of Electrical and Computer Engineering University College of Engineering University of Tehran Tehran Iran Department of Materials Science and Engineering Sharif University of Technology Azadi Ave. P.O. Box 11155-9466 Tehran Iran Research Institute of Petroleum Industry RIPI Tehran14857-33111 Iran Department of Urban and Environmental Engineering Ulsan National Institute of Science and Technology Ulsan44919 Korea Republic of

Surfactants are considered the most influential promoters for accelerating the formation of gas hydrates in gas storage applications. However, their promotion mechanism remains unclear, and the formation of foam during the hydrate dissociation step severely limits hydrate-based gas storage technology. Oleic acid was used as a renewable biomass source in this study to develop a novel biosurfactant capable of enhancing methane hydrate formation. Oleic acid-based promoter (OAP) significantly improved kinetics of methane hydrate formation, and enhanced growth of hydrate crystals. A maximum conversion of 81% and storage capacity of ~151 v/v were achieved in a solution containing 1000 ppm OAP at 9 MPa. Additionally, OAP showed good promotion activity at a lower driving force (7 MPa), resulting in conversion and storage capacity 4.2 times greater than pure water. Moreover, molecular dynamic simulation revealed that the primary mechanism action of OAP is to increase the solubility of methane in an aqueous solution by forming promoter micelles. A gas release simulation for SDS solution generated significant foam, whereas no foam formed when OAP was present. The obtained findings are useful for developing efficient biosurfactants based on vegetable oils and can shed light on the promotion mechanism of promoters. © 2023, The Authors. All rights reserved.

关键词： Gas hydrates

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Nutrient Recovery for Fertilizer Production and Wastewater Treatment for a Circular Economy

ACS Sustainable Resource Management

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ACS Sustainable Resource Management 2024年第4期1卷 787-798页

作者： Mst. Mahmoda Akter Md. Anwar Hosen Brandon H. Gilroyed Shamima Akter Eti Protima Sarker Mohammad Mahbub Kabir Mohammad Mohinuzzaman Department of Environmental Science and Disaster Management Noakhali Science and Technology University Noakhali 3814 Bangladesh Department of Mechanical Engineering Faculty of Science and Technology Sonargaon University Dhaka 1215 Bangladesh School of Environmental Sciences University of Guelph Ridgetown Campus Ridgetown N0P 2C0 Canada Centre for Agricultural Renewable Energy and Sustainability (CARES) University of Guelph Ridgetown Campus Ridgetown N0P 2C0 Canada Fibre & Polymer Research Division Bangladesh Council of Scientific & Industrial Research Dr. Qudrat-E-Khuda Road Dhaka 1205 Bangladesh

The recovery of nutrients, particularly nitrogen (N) and phosphorus (P), from wastewater plays a crucial role in mitigating eutrophication and advancing sustainability. This paper introduces a novel approach for recovering these essential elements from municipal wastewater (MWW) using an innovative composite, calcined magnetic layered double hydroxide/hydroxyapatite (CMLDH-HAP). The adsorbent was synthesized by precipitating hydroxyapatite onto magnetic layered double hydroxides derived from agricultural waste, followed by calcination. The adsorption behaviors, characterized by heterogeneous monolayer chemisorption adsorption, and the underlying mechanisms, including interlayer cation and ligand exchange and surface precipitation, demonstrated sustainable recovery of NH4+-N and P from real wastewater treatment plant effluent in column experiments, with a breakthrough time of 15 min. The N- and P-adsorbed CMLDH-HAP was then utilized as an eco-friendly, slow-release fertilizer to enhance the germination, growth, and blooming of Madagascar periwinkle (Catharanthus roseus). Furthermore, the desorption of N and P using a 0.5 M NaHCO3solution enabled the regeneration of CMLDH-HAP, rendering it suitable for recycling N and P from wastewater. Economic viability considerations explored more cost-effective wastewater treatment options, underscoring the potential of CMLDH-HAP. This study thus presents a sustainable solution that integrates the reuse of agricultural waste, effective wastewater treatment, and the recovery of N and P nutrients as fertilizer sources. Implementing the demonstrated technologies can help minimize the environmental impact of wastewater and promote circular economy principles.

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Salinity Gradient Energy Production by Custom-Made Interpolymer Ion Exchange Membranes Utilized in Reverse Electrodialysis System

SSRN

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SSRN 2022年

作者： Kabay, Nalan Altıok, Esra Kaya, Tuğçe Zeynep Smolinska-Kempisty, Katarzyna Güler, Enver Tomaszewska, Barbara Bryjak, Marek Ege University Faculty of Engineering Chemical Engineering Department Izmir35100 Turkey Wroclaw University of Science and Technology Faculty of Chemistry Department of Process Engineering and Technology of Polymer and Carbon Materials Wroclaw50-370 Poland Atılım University Faculty of Engineering Department of Chemical Engineering Ankara06830 Turkey AGH University of Science and Technology Faculty of Geology Geophysics and Environmental Protection Department of Fossil Fuels Cracow30-059 Poland

Reverse electrodialysis (RED) is one of methods to extract salinity gradient energy between two aqueous solutions with different salt concentrations. In this work, custom-made interpolymer ion exchange membranes were employed in the RED stack. The effects of divalent (Mg2+, Ca2+ and SO42-) and monovalent (Li+, K+ and Cl-) ions in the feed solutions prepared from NaCl salt as a function of such process parameters as number of membrane pairs, flow rate, and salinity ratio on power generation by the RED method were studied. It was shown that the maximum power density of 0.561 W/m2 was reached by using three membrane pairs using 1:45 of salt ratio with a feed flow rate of 120 mL/min using only NaCl salt in the feed solutions. The maximum power density was 0.398 W/m2 at 120 mL/min of the flow rate of the feed solutions composed of 90 wt% NaCl and 10 wt% KCl by using a salt ratio of 1:30 while the lowest power density of 0.246 W/m2 was obtained with a feed flow rate of 30 mL/min in the presence of SO42- ions with a similar salt ratio. Consequently, it was seen that while the presence of divalent ions in NaCl solutions had negative impact on power generation by RED system, the addition of monovalent ions having smaller hydrated radius than that of the Na+ ions contributed positively to the power generation. © 2022, The Authors. All rights reserved.

关键词： Sodium chloride

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Bidirectional relationship between type 2 diabetes mellitus and coronary artery disease:Prospective cohort study and genetic analyses

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Chinese Medical Journal 2024年第5期137卷 577-587页

作者： Wenqiang Zhang Li Zhang Chenghan Xiao Xueyao Wu Huijie Cui Chao Yang Peijing Yan Mingshuang Tang Yutong Wang Lin Chen Yunjie Liu Yanqiu Zou Ling Zhang Chunxia Yang Yuqin Yao Jiayuan Li Zhenmi Liu Xia Jiang Ben Zhang Department of Epidemiology and Biostatistics Institute of Systems EpidemiologyWest China-Peking Union Medical College C.C.Chen Institute of HealthWest China School of Public Health and West China Fourth HospitalSichuan UniversityChengduSichuan 610041China Department of Maternal Child and Adolescent HealthWest China School of Public Health and West China Fourth HospitalSichuan UniversityChengduSichuan 610041China Department of Iatrical Polymer Material and Artificial Apparatus School of Polymer Science and EngineeringSichuan UniversityChengduSichuan 610041China Department of Occupational and Environmental Health West China School of Public Health and West China Fourth HospitalSichuan UniversityChengduSichuan 610041China Department of Nutrition and Food Hygiene West China School of Public Health and West China Fourth HospitalSichuan UniversityChengduSichuan 610041China Department of Clinical Neuroscience Karolinska InstitutetStockholm 17177Sweden

Background:While type 2 diabetes mellitus(T2DM)is considered a putative causal risk factor for coronary artery disease(CAD),the intrinsic link underlying T2DM and CAD is not fully *** aimed to highlight the importance of integrated care targeting both diseases by investigating the phenotypic and genetic relationships between T2DM and ***:We evaluated phenotypic associations using data from the United Kingdom Biobank(N=472,050).We investigated genetic relationships by leveraging genomic data conducted in European ancestry for T2DM,with and without adjustment for body mass index(BMI)(T2DM:N_(case)/N_(control)=74,124/824,006;T2DM adjusted for BMI[T2DM_(adj)BMI]:N_(case)/N_(control)=50,409/523,897)and for CAD(N_(case)/N_(control)=181,522/984,168).We performed additional analyses using genomic data conducted in multiancestry individuals for T2DM(N_(case)/N_(control)=180,834/1,159,055).Results:Observational analysis suggested a bidirectional relationship between T2DM and CAD(T2DM→CAD:hazard ratio[HR]=2.12,95%confidence interval[CI]:2.01–2.24;CAD→T2DM:HR=1.72,95%CI:1.63–1.81).A positive overall genetic correlation between T2DM and CAD was observed(r_(g)=0.39,P=1.43×10^(-75)),which was largely independent of BMI(T2DM_(adj)BMI–CAD:r_(g)=0.31,P=1.20×10^(–36)).This was corroborated by six local signals,among which 9p21.3 showed the strongest genetic ***-trait meta-analysis replicated 101 previously reported loci and discovered six novel pleiotropic *** randomization analysis supported a bidirectional causal relationship(T2DM→CAD:odds ratio[OR]=1.13,95%CI:1.11-1.16;CAD→T2DM:OR=1.12,95%CI:1.07-1.18),which was confirmed in multiancestry individuals(T2DM→CAD:OR=1.13,95%CI:1.10-1.16;CAD→T2DM:OR=1.08,95%CI:1.04-1.13).This bidirectional relationship was significantly mediated by systolic blood pressure and intake of 3-hydroxy-3-methylglutaryl coenzyme A reductase inhibitors,with mediation proportions of 54.1%(95%CI:24.9-83.4%)and 90.4%(95%CI

关键词： Type 2 diabetes mellitus Coronary artery disease Phenotypic association Genetic correlation Mendelian randomization

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Machine Learning Prediction on the Fractional Free Volume of polymer Membranes

SSRN

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SSRN 2022年

作者： Tao, Lei He, Jinlong Arbaugh, Tom McCutcheon, Jeffrey R. Li, Ying Department of Mechanical Engineering University of Connecticut StorrsCT06269 United States Department of Physics Wesleyan University MiddletownCT06459 United States Department of Chemical & Biomolecular Engineering Center for Environmental Sciences and Engineering University of Connecticut StorrsCT06269 United States Polymer Program Institute of Materials Science University of Connecticut StorrsCT06269 United States Department of Mechanical Engineering University of Wisconsin-Madison MadisonWI53706 United States

Fractional free volume (FFV) characterizes the microstructural level features of polymers and affects their properties including thermal, mechanical, and separation performance. Experimental measurements and theoretical analyses have been used to quantify the FFV of polymers, but challenges remain because of their limitations. Experimental measurements are laborious and based on semi-empirical equations, while Bondi’s group contribution theory involves ambiguities like the determination of van der Waals volume and the choice of factor values in the theoretical equation. To efficiently evaluate the FFV of polymers, this study utilizes high-throughput molecular dynamics (MD) simulations to build a large dataset regarding polymer’s FFV. Based on this large dataset, we further build machine learning (ML) models to establish the composition-structure relation. Inspired by group contribution theory which correlates polymer’s functional groups to FFV, our ML models correlate polymer’s sub-structures or physico-chemical indexes to FFV. Our study first benchmarks the MD simulation protocol to obtain reliable FFV of polymers and then carries out high-throughput MD simulations for more than 6,500 homopolymers and 1,400 polyamides. Such a large and diverse dataset makes the well-trained ML models more generalizable, compared with the group contribution theory. The efficiency of a feed-forward neural network model is further demonstrated by applying it to a hypothetical polyimide dataset of more than 8 million chemical structures. The predicted FFVs of hypothetical polyimides are further validated by MD simulations. The obtained FFVs of the 8 million polymers, plus their previously reported gas separation performances, demonstrate the promising capability of ML virtual screening for the discovery of polymer membranes with exceptional permeability/selectivity. © 2022, The Authors. All rights reserved.

关键词： Molecular dynamics

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High‑Performance Thick Cathode Based on Polyhydroxyalkanoate Binder for Li Metal Batteries

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Advanced Fiber Materials 2024年第1期6卷 214-228页

作者： Dong Hyuk Kang Minhyuck Park Jeonghun Lee Chan Yeol Kim Jimin Park Youn‑Ki Lee Jong Chan Hyun Son Ha Jin Hwan Kwak Juhee Yoon Hyemin Kim Hyun Soo Kim Do Hyun Kim Sangmin Kim Ji Yong Park Robin Jang Seung Jae Yang Hee‑Dae Lim Se Youn Cho Hyoung‑Joon Jin Seungjin Lee Yunil Hwang Young Soo Yun KU‑KIST Graduate School of Converging Science and Technology Korea University145 Anam‑roSeongbuk‑guSeoul 02841South Korea Carbon Composite Materials Research Center Korea Institute of Science and Technology(KIST)92 Chundong‑roBongdong‑eupWanju‑gunJeollabuk‑do 55324South Korea Energy Storage Research Center Korea Institute of Science and Technology(KIST)514‑gil Hwaraong‑roSeoul 02792South Korea Program in Environmental and Polymer Engineering Inha University100 Inha‑ro Michuhol‑guIncheon 22212South Korea Advanced Analysis Data Center Korea Institute of Science and Technology(KIST)514‑gil Hwaraong‑roSeoul 02792South Korea Advanced Nanohybrids Laboratory Department of Chemistry and Chemical EngineeringInha University100 Inha‑roMichuhol‑guIncheon 22212South Korea CJ CheilJedang Corporation 55 Gwanggyo‑ro 42Beon‑gilYeongtong‑guSuwon 16495South Korea Department of Chemical Engineering Hanyang University222 Wangsimni‑roSeongdong‑guSeoul 04763South Korea Department of Integrative Energy Engineering Korea University145 Anam‑roSeongbuk‑guSeoul 02841South Korea

Thick cathodes can overcome the low capacity issues,which mostly hamper the performance of the conventional active cathode materials,used in rechargeable Li ***,the typical slurry-based method induces cracking and flaking during the fabrication of thick *** addition,a significant increase in the charge-transfer resistance and local cur-rent overload results in poor rate capabilities and cycling stabilities,thereby limiting electrode *** this study,a synergistic dual-network combination strategy based on a conductive nanofibrillar network(CNN)and a nano-bridging amor-phous polyhydroxyalkanoate(aPHA)binder is used to demonstrate the feasibility of constructing a high-performance thick *** CNN and aPHA dual network facilitates the fabrication of a thick cathode(≥250μm thickness and≥90 wt%active cathode material)by a mass-producible slurry *** thick cathode exhibited a high rate capability and excel-lent cycling *** addition,the thick cathode and thin Li metal anode pair(Li//t-NCM)exhibited an optimal energy performance,affording high-performance Li metal batteries with a high areal energy of~25.3 mW h cm^(-2),a high volumetric power density of~1720 W L^(-1),and an outstanding specific energy of~470 W h kg^(-1)at only 6 mA h cm^(-2).

关键词： Thick cathode Polyhydroxyalkanoate binder Nano-bridging Conductive nano-fibrillar network Lithium metal battery

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Mapping Hydrogen Evolution Activity Trends of V-based A15 Superconducting Alloys

arXiv

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arXiv 2024年

作者： Yu, Peifeng Zhan, Jie Zhang, Xiaobing Wang, Kangwang Zeng, Lingyong Li, Kuan Zhang, Chao Li, Longfu Liang, Ying Yan, Kai Sun, Yan Luo, Huixia School of Materials Science and Engineering State Key Laboratory of Optoelectronic Materials and Technologies Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices Key Lab of Polymer Composite & Functional Materials Sun Yat-Sen University Guangzhou510275 China Beijing Advanced Innovation Center for Materials Genome Engineering State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing100083 China Basic Course Department Guangzhou Maritime University Guangzhou510725 China School of Environmental Science and Engineering Sun Yat-Sen University Guangzhou510275 China Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Shenyang110016 China School of Materials Science and Engineering University of Science and Technology of China Shenyang110016 China

Exploring high-efficiency and low-cost electrocatalysts is valuable for water-splitting technologies. Recently, Si-group compounds have attracted increasing attention in electrocatalysis, considering the abundant Si-group elements on Earth. However, Si-group compounds for HER electrocatalysis have not been systematically studied. In this study, we unveil the activity trends of non-noble metal catalyst A15-type V3M (i.e., V3Si, V3Ge, and V3Sn) superconductors and show that V3Si is the most efficient HER catalyst because of the high electronic conductivity and suitable d-band center. Among them, the V3Si only requires 33.4 mV to reach 10 mA cm-2, and only 57.6 mV and 114.6 mV are required to attain a high current density of 100 mA cm−2 and 500 mA cm−2, respectively. These low overpotentials are close to the 34.3 mV at 10 mA cm−2 of state-of-art Pt/C (20 %) but superior to 168.5 mV of Pt/C (20 %) at 100 mA cm-2. Furthermore, the V3Si illustrates exceptional durability with no obvious decay in the 120 h at the different current densities (i.e., 10 - 250 mA cm−2). The excellent HER activity of V3Si alloy can be ascribed to the synergies of superior electronic conductivity and suitable d-band center. Moreover, DFT calculations reveal that |ΔGH*| is decreased after introducing the V to Si. Beyond offering a stable and high-performance electrocatalyst in an acidic medium, this work inspires the rational design of desirable silicide electrocatalysts. Copyright © 2024, The Authors. All rights reserved.

关键词： Hydrogen

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Evaluating Cost & Safety Trade-Off in High-Pressure Proton Exchange Membrane Electrolyzer Cells (Pemecs)

SSRN

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SSRN 2023年

作者： Dang, Jing Qi, Meng Xu, Chi-Min Feng, Wei Liu, Yi Qingdao266580 China Department of Safety Health and Environmental Engineering National Yunlin University of Science and Technology Yunlin64002 Taiwan State Key Laboratory of Fluorinated Functional Membrane Materials Zibo256401 China Shandong Dongyue Polymer Material Co. Ltd. Zibo256401 China

Proton exchange membrane electrolysis cells (PEMECs) offer a pathway for green hydrogen production but is limited by high costs. We noted that high-pressure PEMECs reduce hydrogen transportation expenses nevertheless enhance hydrogen cross-membrane transfer. The absence of adaptive electrolysis reaction safety scoring approach takes challenge for multi-objective optimization. Here, we designed inherent safety index and developed a first-principle model with process simulation to reveal the trade-off between safety performance and economic performance, subsequently tried to optimize by adjusting the operating parameters. Cost analyses show hydrogen production rates between 2 to 10 $/Nm3, consistent with recent studies. The results showed a decrease in cost, but a fluctuation in safety scores with increasing pressure, and Pareto trade-off front exhibited a spiral distribution influenced by membrane thickness, cathode pressure, and current density. In addition, Convex Hull algorithm have obvious advantages over the Non-dominated Sorting Genetic Algorithm II (NSGA-II) algorithm in terms of trade-off solution performance. © 2023, The Authors. All rights reserved.

关键词： Multiobjective optimization

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