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Swelling and dissolution behaviors of cellulose in phosphate-based ionic liquids-H2O binary systems: In-situ observation and molecular dynamics simulation

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Journal of Molecular Liquids 2024年 415卷

作者： Cao, Ruimei Long, Yan Li, Tiancheng Lv, Wanxue Wu, Huizheng Wang, Binqi Song, Yuting Gao, Hongshuai Nie, Yi School of Chemical Engineering Zhengzhou University Zhengzhou450001 China Zhengzhou Institute of Emerging Industrial Technology Longzihu New Energy Laboratory Zhengzhou450046 China Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

Swelling and dissolution of cellulose in ionic liquids (ILs) as the pretreatment processes are key steps for the high-value conversion and utilization of cellulose. However, the molar ratio of H2O to ILs has a significant effect on the swelling and dissolution of cellulose, and its molecular-scale mechanism is still unclear, which limits screening out the suitable ILs and recovery of ILs from coagulation bath in the spinning process. Herein, three phosphate-based ILs were chosen to couple with water as solvents for swelling and dissolution of cellulose by combining in-situ observation and molecular dynamics (MD) simulation. The results show that the redissolution time of swollen cellulose is greatly reduced, especially [Emim]DEP-H2O has the best swelling and dissolution performance for cellulose due to its high β value and low viscosity. Meanwhile, when the molar ratio of IL to H2O was more than 1: -1, the IL-H2O system still has the ability to dissolve cellulose. While with the molar ratio further decreased, cellulose was no longer dissolved and began to swell, and the fiber diameter obtained the maximum swelling rate with 40.1% at a molar ratio of 1:3. Moreover, MD simulation was used to calculate the interaction between IL/water/cellulose, which further illustrated that the combination of IL with water molecular has a significant influence on the behavior of cellulose in IL-H2O systems at the molecular scale. Thus, the potential swelling and dissolution mechanism of cellulose in ILs-H2O binary systems was proposed based on experimental and simulation results. Furthermore, the characterization results of swollen cellulose indicate that the crystal structure and degree of polymerization (DP) were almost unchanged, but the specific surface area and pore size increased significantly, and the thermal stability and heat absorption were decreased, all the results prove that the swelling process increased the accessibility of cellulose and benefited to the subsequent dis

关键词： Spinning (fibers)

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Triple the steady-state reaction rate by decorating the In_(2)O_(3)surface with SiO_(x)for CO_(2)hydrogenation

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Journal of Energy Chemistry 2024年第8期95卷 96-105,I0003页

作者： Hao Wang Chun Yang Xiaoyan Yu Mingrui Wang Runze Yang Xiaowa Nie Ben Hang Yin Alex C.K.Yip Chunshan Song Guanghui Zhang Xinwen Guo State Key Laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsPSU-DUT Joint Center for Energy ResearchSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Department of Chemistry the Chinese University of Hong KongHong Kong 999077China Paihau-Robinson Research Institute the MacDiarmid Institute for Advanced Materials and NanotechnologyVictoria University of WellingtonWellington 6012New Zealand Department of Chemical and Process Engineering The University of CanterburyChristchurch 8041New Zealand

Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction *** on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In_(2)O_(3)nanoparticles by the surface decoration with highly dispersed silica species(SiO_(x)).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability originated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited CO_(2)conversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in CO_(2)*** steady-state activity was also achieved on Pd-modified *** to the traditional Pd/In_(2)O_(3)catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In_(2)O_(3)was enhanced by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform *** work provides a promising method to design new In_(2)O_(3)-based catalysts with improved activity and stability in CO_(2)hydrogenation.

关键词： CO_(2)hydrogenation In_(2)O_(3)sintering Dynamic structural evolution Surface SiO_(x)modification DFT simulations

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Metabolic Mechanism of P-Cresol Biodegradation by Bacillus Subtilis Zw: Coexistence of Diverse Metabolic Pathways

SSRN

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SSRN 2024年

作者： Wang, Xueting Liu, Shihao Ding, Xiaoke Zhang, Lele Lv, Xueru Li, Jie Song, Caihong Zhang, Chen Wang, Shenghui College of Life Science Liaocheng University Liaocheng252059 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

The aromatic compound p-cresol is a notorious industrial pollutant characterized by its high toxicity, persistence and bioaccumulation within higher organisms. A thorough understanding of the microbial metabolic pathways involved in p-cresol degradation is critical for the design and optimization of microbial wastewater treatment systems. Despite numerous studies on the degradation pathways of p-cresol by various microbial species, the metabolic diversity within a single strain remains largely unexplored. This study investigated the metabolic mechanism of p-cresol in Bacillus subtilis ZW, a bacterium capable of degrading p-cresol. Through LC-MS analysis, we identified twelve distinct metabolic intermediates in the culture of strain ZW, leading to the proposal of three plausible degradation pathways. These include methyl hydroxylation, direct aromatic ring hydroxylation, and phosphorylation of the hydroxyl group, and all of which may concurrently contribute to p-cresol biodegradation by strain ZW. Further study showed that the genome of strain ZW harbored 47 coding genes associated with the degradation of p-cresol and its structural analogs, underscoring the metabolic versatility of this strain and its potential for xenobiotic biodegradation. These findings contribute valuable insights into the biodegradation mechanisms of pollutants. Under optimal degradation conditions of 35 °C and pH 7.0, strain ZW demonstrated the capacity to metabolize 27.5% of p-cresol (10 mg/L) in minimal salt media within a week, and was capable of completely degrading 10 mg/L p-cresol in wastewater within five days. The potential utility of strain ZW in the bioremediation of p-cresol and other aromatic compounds is thus evident. © 2024, The Authors. All rights reserved.

关键词： Aromatization

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Strategic design and fabrication of MXenes-Ti_(3)CNCl_(2)@CoS_(2) core-shell nanostructure for high-efficiency hydrogen evolution

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Nano Research 2022年第7期15卷 5977-5986页

作者： Jizhou Jiang Saishuai Bai Meiqing Yang Jing Zou Neng Li Jiahe Peng Haitao Wang Kun Xiang Song Liu Tianyou Zhai School of Environmental Ecology and Biological Engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan 430205China College of Life and Environmental Science Hunan University of Arts and ScienceChangde 415000China Key Laboratory of Rare Mineral Ministry of Natural ResourcesGeological Experimental Testing Center of Hubei ProvinceWuhan 430034China State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China Institute of Chemical Biology and Nanomedicine(ICBN) State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

CoS_(2) is considered to be a promising electrocatalyst for hydrogen evolution reaction(HER).However,its further widespread applications are hampered by the unsatisfactory activity due to relatively high chemisorption energy for hydrogen ***,theoretical predictions of first-principles calculations reveal that the introduction of a Cl-terminated MXenes-Ti_(3)CNCl_(2) can significantly reduce the HER potential of CoS_(2)-based materials and the Ti_(3)CNCl_(2)@CoS_(2) core–shell nanostructure has Gibbs free energy of hydrogen adsorption(|ΔGH|)close to zero,much lower than that of the pristine CoS_(2) and Ti_(3)CNCl_(2).Inspired by the theoretical predictions,we have successfully fabricated a unique Ti_(3)CNCl_(2)@CoS_(2) core–shell nanostructure by ingeniously coupling CoS_(2) with a Cl-terminated MXenes-Ti_(3)CNCl_(2).Interface-charge transfer between CoS_(2) and Ti_(3)CNCl_(2) results in a higher degree of electronic localization and a formation of chemical ***,the Ti_(3)CNCl_(2)@CoS_(2) core–shell nanostructure achieves a significant enhancement in HER activity compared to pristine CoS_(2) and Ti_(3)CNCl_(2).Theoretical calculations further confirm that the partial density of states of CoS_(2) after hybridization becomes more non-localized,and easier to interact with hydrogen ions,thus boosting HER *** this work,the success of oriented experimental fabrication of high-efficiency Ti_(3)CNCl_(2)@CoS_(2) electrocatalysts guided by theoretical predictions provides a powerful lead for the further strategic design and fabrication of efficient HER electrocatalysts.

关键词： theoretical predictions Ti_(3)CNCl_(2)@CoS_(2)core-shell nanostructure electronic non-localization hydrogen evolution

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Developing hierarchical CdS/NiO hollow heterogeneous architectures for boosting photocatalytic hydrogen generation

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Nano Research 2022年第3期15卷 2003-2012页

作者： Chonghai Deng Fan Ye Tao Wang Xiaohui Ling Lulu Peng Hong Yu Kangzhe Ding Hanmei Hu Qiang Dong Huirong Le Yongsheng Han School of Energy Materials and Chemical Engineering Hefei UniversityHefei 230601China Anhui Province Key Laboratory of Advanced Building Materials Anhui Jianzhu UniversityHefei 230601China The Future Lab Tsinghua UniversityBeijing 100084China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

The hierarchical binary CdS/NiO hollow heterogeneous architectures(HHAs)with p–n heterojunction are constructed by a facile microwave-assisted wet chemical process for high-efficient photocatalytic hydrogen evolution reaction(HER)from *** as-designed CdS/NiO HHAs are composed of hexagonal n-type CdS nanoparticles with a size in the range of 20–40 nm attaching to cubic p-type NiO hollow microspheres(HMSs)which are aggregates of porous nanoplates with a thickness of about 20 *** photocatalytic water splitting over CdS/NiO HHAs is significantly increased under simulated solar irradiation,among which the most active sample of CdS/NiO-3(the mass ratio of CdS to NiO is 1:3)exhibits the fastest photocatalytic HER rate of 1.77 mmol∙g^(−1)∙h^(−1),being 16.2 times than that of pure *** boosted photocatalytic HER could be attributed to the synergistic effect on the proportional p–n heterojunction with special hierarchical hollow and porous morphology,an enhancement of visible light absorption,and an improvement of photoinduced charge separation as well as the photo-stability given by the composite *** work shows a viable strategy to design the heterojunction with special morphology for the efficient hydrogen generation by water splitting utilizing solar energy.

关键词： CdS nanoparticls NiO hollow microspheres p-n heterojunction hierarchical structure photocatalytic hydrogen evolution

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Facile Fabrication of Core-Shell Structure Fe_(3)O_(4)@C Nanodots for Enhanced Lithium-Sulfur Batteries

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Acta Metallurgica Sinica(English Letters) 2021年第3期34卷 410-416页

作者： Xiang-Rui He Yu-Jiao Zhang Li-Fan Yang Ji-Lu Zhao Hong-Tai Li Yi-Bo Gao Bao Wang Xiao-Dong Guo School of Chemical Engineering Sichuan UniversityChengdu 610065China State Key Laboratory of Biochemical Engineering.Instituteof Process Engineering Chinese Academy of SciencesBeijing 100190China School of Chemistry Sun Yat-Sen UniversityGuangzhou 510275China

Lithium sulfur battery(LSB) is widely considered as a next-generation battery system due to its high theoretical energy density of 2567 Wh ***,several inherent issues obstruct the business application of *** address these issues,we assemble core-shell structure Fe_(3)O_(4)@C nanodots with 5 nm diameter as a valid sulfur host via a convenient organic pyrolysis treatment followed by *** nanosized Fe3O4 particles could expose more chemisorption sites and inhibit the polysulfides ***,the carbon layer could not only increase the conductivity but also ensure structural integrity during cyclic ***,the mesoporous channels around Fe_(3)O_(4)@C could supply sufficient space to load sulfur and physically restrict the shuttle of ***,the resultant S/Fe_(3)O_(4)@C cathode shows a highly initial capacity of 1089 mAh g^(-1) at 0.2 C,even retains 655 mAh g^(-1) over 200 cycles at 1 C.

关键词： Fe(3)O_(4) Nanodots Cathode Lithium–sulfur batteries

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Core-shell gold-copper nanoparticles:Evolution of copper shells on gold cores at different gold/copper precursor ratios

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Chinese Journal of Structural Chemistry 2023年第11期42卷 32-39页

作者： Shaonan Tian Yu Zhang Qing Zeng Junyu Zhong Hui Liu Lin Xu Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China State Key Laboratory of Bio-fibers and Eco-textiles Qingdao UniversityQingdao266071China School of Chemistry and Materials Science Jiangsu Key Laboratory of New Power BatteriesJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjing210023China

Core-shell nanostructures usually exhibit tunable catalytic properties in comparison with their single core or shell counterpart due to electronic interaction and lattice strain between the core and shell ***,we report the intriguing evolution of copper(Cu)shells on the gold(Au)cores at different Au/Cu precursor ratios during the synthesis of core-shell Au-Cu nanoparticles at an organic medium via seed-mediated growth *** brief,at relatively low Cu ratios,quasi-spherical Au-Cu nanoparticles with conventional core-shell structures are the majority products,in which the Cu shell thickness increases with the increase of Cu precursor *** dif-ference is that at high Cu ratios,the Cu shells no longer increase their thickness,but evolve into a dendritic ***,the core-shell Au-Cu nanoparticles with dendritic Cu shells could be transformed into interesting Au-Cu cage-bell structures after a ripening process at elevated ***,through galvanic replacement reaction with Pt precursors,the thin Cu shells could be converted into CuPt alloy shells on the Au cores,which exhibit enhanced activity towards methanol oxidation reaction with satisfactory durability,in comparison with that of commercial Pt/C catalysts.

关键词： Core-shell nanostructure Seed-mediated growth Electronic interaction Lattice strain Methanol oxidation reaction

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Conjugated microporous polymers-scaffolded enzyme cascade systems with enhanced catalytic activity

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Chinese Journal of Catalysis 2024年第8期63卷 213-223页

作者： Zhenhua Wu Jiafu Shi Boyu Zhang Yushuai Jiao Xiangxuan Meng Ziyi Chu Yu Chen Yiran Cheng Zhongyi Jiang School of Environmental Science and Engineering Tianjin UniversityTianjin 300072China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China College of Chemical Engineering Fuzhou UniversityFuzhou 350108FujianChina Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207FujianChina

Enhancing catalytic activity of multi-enzyme in vitro through substrate channeling effect is promis-ing yet ***,conjugated microporous polymers(CMPs)-scaffolded integrated en-zyme cascade systems(I-ECSs)are constructed through co-entrapping glucose oxidase(GOx)and horseradish peroxidase(HRP),in which hydrogen peroxide(H_(2)O_(2)) is the intermediate *** interplay of low-resistance mass transfer pathway and appropriate pore wall-H_(2)O_(2) interactions facilitates the directed transfer of H_(2)O_(2),resulting in 2.4-fold and 5.0-fold elevation in catalytic activ-ity compared to free ECSs and separated ECSs,*** substrate channeling effect could be regulated by altering the mass ratio of GOx to ***,I-ECSs demonstrate excellent stabili-ties in harsh environments and multiple recycling.

关键词： Biocatalysis Immobilization Enzyme cascade system Substrate channeling effect Conjugated microporous polymers

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Bioplastic production in terms of life cycle assessment:A state-of-theart review

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Environmental Science and Ecotechnology 2023年第3期15卷 14-34页

作者： Sameh Samir Ali Esraa A.Abdelkarim Tamer Elsamahy Rania Al-Tohamy Fanghua Li Michael Kornaros Antonio Zuorro Daochen Zhu Jianzhong Sun Biofuels Institute School of the Environment and Safety EngineeringJiangsu UniversityZhenjiang212013PR China Botany Department Faculty of ScienceTanta UniversityTanta31527Egypt State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbinHeilongjiang Province150090China Laboratory of Biochemical Engineering&Environmental Technology(LBEET) Department of Chemical EngineeringUniversity of Patras26504PatrasGreece Department of Chemical Engineering Materials and EnvironmentSapienza University00184RomeItaly

The current transition to sustainability and the circular economy can be viewed as a socio-technical response to environmental impacts and the need to enhance the overall performance of the linear production and consumption *** concept of biowaste refineries as a feasible alternative to petroleum refineries has gained *** has become an important raw material source for developing bioproducts and ***,effective environmental biowaste management systems for the production of bioproducts and biofuels are crucial and can be employed as pillars of a circular ***,typically plastics manufactured from bio-based polymers,stand to contribute to more sustainable commercial plastic life cycles as part of a circular economy in which virgin polymers are made from renewable or recycled raw *** frameworks and strategies are utilized to model and illustrate additional patterns in fossil fuel and bioplastic feedstock prices for various governments'long-term *** review paper highlights the harmful impacts of fossil-based plastic on the environment and human health,as well as the mass need for eco-friendly alternatives such as biodegradable *** new types of bioplastics derived from renewable resources(e.g.,biowastes,agricultural wastes,or microalgae)and choosing the appropriate end-of-life option(e.g.,anaerobic digestion)may be the right direction to ensure the sustainability of bioplastic *** regulation and financial incentives are still required to scale from niche polymers to large-scale bioplastic market applications with a truly sustainable impact.

关键词： Biowaste Bioeconomy Bioplastic Life cycle assessment Biofuel

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Ordered mesoporous carbon spheres assisted Ru nanoclusters/RuO_(2) with redistribution of charge density for efficient CO_(2) methanation in a novel H2/CO_(2)fuel cell

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Journal of Energy Chemistry 2022年第9期31卷 116-124,I0004页

作者： Yan Liu Tao Zhang Chao Deng Shixiu Cao Xin Dai Shengwu Guo Yuanzhen Chen Qiang Tan Haiyan Zhu Sheng Zhang Yongning Liu State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049ShaanxiChina Department of Chemical and Biochemical Engineering RutgersThe State University of New JerseyPiscataway 08854New JerseyUnited States Chongqing University Key Laboratory of Micro/Nano Materials Engineering and Technology Chongqing University of Arts and SciencesChongqing 402160China Institute of Modern Physics Northwest UniversityShaanxi Key Laboratory for Theoretical Physics FrontiersXi’an 710069ShaanxiChina Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Efficiently reducing carbon dioxide(CO_(2))into carbon chemicals and fuels is highly desirable due to the rapid growth of atmospheric CO_(2)*** prior work,we described a unique H/CO_(2)fuel cell driven by low-valued waste heat,which not only CO_(2)nverts CO_(2)to methane(CH_(4))but also outputs electrical energy,yet the CO_(2)reduction rate needs to be urgently ***,a novel Ru-RuOcatalyst with heterostructure was grafted on mesoporous carbon spheres by in situ partially reducing RuOinto ultrasmall Ru clusters(~1 nm),in which heteroatom-doped carbon spheres as a matrix with excellent CO_(2)nductivity and abundant pores can not only easily CO_(2)nfine the formation of Ru nanocluster but also are beneficial to the exposed active sites of Ru CO_(2)mplex and the mass ***_(2)mpared to pure RuOnanoparticles supported on carbon spheres,our CO_(2)mposite catalyst boosts the CO_(2) nversion rate by more than 5-fold,reaching a value of 382.7μmol gcat.h-1at 170℃.Moreover,a decent output power density of 2.92 W mwas obtained from this H2/CO_(2)fuel cell using Ru-RuOembedded carbon spheres as a cathode *** Ru-RuOheterostructure can modify the adsorption energy of CO_(2)and induce the redistribution of charge density,thus boosting CO_(2)reduction *** work not only offers an efficient catalyst for this novel H_(2)/CO_(2)fuel cell but also presents a facile method to prepare Ru nanoclusters.

关键词： CO_(2)methanation Fuel cell Generating electricity Ru nanocluster/RuO_(2)hybrid Ordered mesoporous carbon spheres

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