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Enhanced direct gaseous CO_(2) fixation into higher bio-succinic acid production and selectivity

Journal of Environmental Sciences 2024年第9期143卷 164-175页

作者： Ziyi Yang Wanling Wu Qing Zhao Irini Angelidaki Samuel Gyebi Arhin Dongliang Hua Yuxiao Zhao Hangyu Sun Guangqing Liu Wen Wang Biomass energy and Environmental engineering Research Center Beijing University of Chemical TechnologyBeijing 100029China College of chemical engineering Beijing University of Chemical TechnologyBeijing 100029China department of chemical and Biochemical Environmental engineering Technical University of DenmarkDK-2800Kgs LyngbyDenmark energy Research Institute Qilu University of Technology(Shandong Academy of Sciences)Shandong Provincial Key Laboratory of Biomass Gasification TechnologyJinan 250014China

Utilizing CO_(2)for bio-succinic acid production is an attractive approach to achieve carbon capture and recycling(CCR)with simultaneous production of a useful platform chemical.Actinobacillus succinogenes and Basfia succiniciproducens were selected and investigated as microbial catalysts.Firstly,the type and concentration of inorganic carbon concentration and glucose concentration were evaluated.6 g C/L MgCO_(3)and 24 g C/L glucose were found to be the optimal basic operational conditions,with succinic acid production and carbon yield of over 30 g/L and over 40%,respectively.Then,for maximum gaseous CO_(2)fixation,carbonate was replaced with CO_(2)at different ratios.The“less carbonate more CO_(2)”condition of the inorganic carbon source was set as carbonate:CO_(2)=1:9(based on the mass of carbon).This condition presented the highest availability of CO_(2)by well-balanced chemical reaction equilibrium and phase equilibrium,showing the best performance with regarding CO_(2)fixation(about 15 mg C/(L·hr)),with suppressed lactic acid accumulation.According to key enzymes analysis,the ratio of phosphoenolpyruvate carboxykinase to lactic dehydrogenase was enhanced at high ratios of gaseous CO_(2),which could promote glucose conversion through the succinic acid path.To further increase gaseous CO_(2)fixation and succinic acid production and selectivity,stepwise CO_(2)addition was evaluated.50%-65%increase in inorganic carbon utilization was obtained coupled with 20%-30%increase in succinic acid selectivity.This was due to the promotion of the succinic acid branch of the glucose metabolism,while suppressing the pyruvate branch,along with the inhibition on the conversion from glucose to lactic acid.

关键词： Succinic acid CO_(2) fixation Actinobacillus succinogenes Basfia succiniciproducens Lactic acid

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Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer

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Nano-Micro Letters 2024年第7期16卷 59-73页

作者： Leqi Zhao Yijun Zhong Chencheng Cao Tony Tang Zongping Shao WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWA 6102Australia

The pursuit of safer and high-performance lithium-ion batteries(LIBs)has triggered extensive research activities on solid-state batteries,while challenges related to the unstable electrode-electrolyte interface hinder their practical implementation.Polymer has been used extensively to improve the cathode-electrolyte interface in garnet-based all-solid-state LIBs(ASSLBs),while it introduces new concerns about thermal stability.In this study,we propose the incorporation of a multi-functional flame-retardant triphenyl phos-phate additive into poly(ethylene oxide),acting as a thin buffer layer between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and garnet electro-lyte.Through electrochemical stability tests,cycling performance evaluations,interfacial thermal stability analysis and flammability tests,improved thermal stability(capacity retention of 98.5%after 100 cycles at 60℃,and 89.6%after 50 cycles at 80℃)and safety characteristics(safe and stable cycling up to 100℃)are demonstrated.Based on various materials characterizations,the mechanism for the improved thermal stability of the interface is proposed.The results highlight the potential of multi-functional flame-retardant additives to address the challenges associated with the electrode-electrolyte interface in ASSLBs at high temperature.Efficient thermal modification in ASSLBs operating at elevated temperatures is also essential for enabling large-scale energy storage with safety being the primary concern.

关键词： Solid-state battery Cathode electrolyte interlayer Flame-retardant additive Cycling stability Interfacial stability

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Synergistic effect of adsorption and photocatalytic degradation of oilfield-produced water by electrospun photocatalytic fibers of Polystyrene/Nanorod-Graphitic carbon nitride

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Journal of Environmental Sciences 2024年第7期141卷 287-303页

作者： Parisa Azmoon Mehrdad Farhadian Alireza Pendashteh Amir H.Navarchian department of chemical engineering Faculty of EngineeringUniversity of IsfahanIsfahanIran department of chemical engineering Faculty of EngineeringUniversity of GuilanRashtIran department of Water and Environmental engineering Caspian Sea Basin Research CenterUniversity of GuilanRashtIran

Graphitic carbon nitride with nanorod structure(Nr-GCN)was synthesized using melamine as a precursor without any other reagents by hydrothermal pretreatment method.XRD,FTIR,SEM,N_(2)adsorption-desorption from BET,UV-Vis DRS spectroscopy,and photoluminescence were used to characterize the prepared samples.Also,the photoelectrochemical behavior of nanoparticles was studied by photocurrent transient response and cyclic voltammetry analysis.Polystyrene(PS)fibrous mat was fabricated by electrospinning technique and used as a support for the stabilization of the nanoparticles.The performance of the synthesized nanoparticles and photocatalytic fibers(PS/Nr-GCN)was evaluated in oilfield-produced water treatment under visible light irradiation.During this process,oil contaminants were adsorbed by hydrophobic polystyrene fibers and simultaneously degraded by Nr-GCN.The removal efficiency of chemical oxygen demand(COD)has been obtained 96.6%and 98.4%by Nr-GCN and PS/Nr-GCN,respectively,at the optimum conditions of pH4,photocatalyst dosage 0.5 g/L,COD initial concentration 550 mg/L,and illumination time 150 min.The gas chromatography-mass spectroscopy analysis results showed 99.3%removal of total petroleum hydrocarbons using photocatalytic fibers of PS/Nr-GCN.The results demonstrated that the GCN has outstanding features like controllable morphology,visible-light-driven,and showing high potential in oily wastewater remediation.Moreover,the synergistic effect of adsorption and photocatalytic degradation is an effective technique in oilfield-produced water treatment.

关键词： Graphitic carbon nitride(GCN) Nanorod structure Polystyrene fibrous mat Photocatalytic fibers Oilfield-produced water(OPW)

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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of energy Chemistry 2024年第8期95卷 20-28页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key Lab of Fine chemicals Liaoning Key Lab for Energy Materials and Chemical Engineering Frontier Science Center for Smart Materials School of Chemical EngineeringDalian University of Technology Liaoning Key Lab for energy Materials and chemical engineering Frontier Science Center for Smart Materials School of Chemistry Dalian University of Technology State Key Laboratory of chemical Resource engineering College of Chemical Engineering Beijing University of Chemical Technology

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon materials. However, the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging task. Herein, the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center calculations. To experimentally verify this, the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P), subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO) via π-π interactions. The multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-ordered π electron delocalization system as conductive network. The defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%, superior to the Pt reference(7.97%). Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates, thus enhancing the electrocatalytic activity of the catalyst. This work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Carbon quantum dots Defect engineering Electrocatalytic activity Pentagon carbon Triiodide reduction

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Migration and transformation of Pb,Cu,and Zn during co-combustion of high-chlorine-alkaline coal and Si/Al dominated coal

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Journal of Environmental Sciences 2024年第7期141卷 26-39页

作者： Jiangze Luo Qiwei Yang Jianqiao Wang Boxiong Shen Zhuozhi Wang Qiqi Shi Zhong Zhao Chao Huang Jie Xu Tianjin Key Laboratory of Clean energy and Pollution Control School of Energy and Environmental EngineeringHebei University of TechnologyTianjin 300103China School of chemical engineering Hebei University of TechnologyTianjin 300103China

Shaerhu(SEH)coal is abundant in Xinjiang,China.The utilization of SEH suffers from severe ash deposition,slagging,and fouling problems due to its high-chlorine-alkaline characteristics.The co-combustion of high-alkaline coal and other type coals containing high Si/Al oxides has been proven to be a simple and effective method that will alleviate ash-related problems,but the risk of heavy metals(HMs)contamination in this process is nonnegligible.Hence,the volatilization rates and chemical speciation of Pb,Cu,and Zn in co-combusting SEH and a high Si/Al oxides coal,i.e.,Yuanbaoshan(YBS)coal were investigated in this study.The results showed that the addition of SEH increased the volatilization rates of Pb,Cu,and Zn during the co-combustion at 800℃from 23.70%,23.97%,and 34.98%to 82.31%,30.01%,and 44.03%,respectively,and promoted the extractable state of Cu and Zn.In addition,the interaction between SEH and YBS inhibited the formation of the Pb residue state.SEM-EDS mapping results showed that compared to Zn and Cu,the signal intensity of Pb was extremely weak in regions where some of the Si and Al signal distributions overlap.The DFT results indicated that the O atoms of the metakaolin(Al_(2)O_(3)·2SiO_(2))(001)surface were better bound to the Zn and Cu than Pb atoms after adsorption of the chlorinated HMs.These results contribute to a better understanding of the effects of high-alkaline coal blending combustion on Pb,Cu,and Zn migration and transformation.

关键词： Heavy metals High-chlorine-alkaline coal Coal blending combustion Density functional theory

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Recent advances in the microfluidic generation of shape-controllable hydrogel microparticles and their applications

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Green chemical engineering 2024年第1期5卷 16-30页

作者： Yingzhe Liu Zhuo Chen Jianhong Xu The State Key Lab of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Hydrogel microparticles,generally accepted as significant green materials,have been widely used in chemical,biological,and biomedical fields owing to their excellent biocompatibility,biodegradability,and noncytotoxicity.Among these,non-spherical hydrogel microparticles with diverse shape anisotropy have great potential in applications such as drug delivery,cellular interaction,micromotors,etc.Benefiting from their shapes,their functionalities in such fields cannot be satisfied by the typical spherical types.Recently,microfluidics with precise control and domination of fluids at microflow sizes has emerged as a powerful method for synthesizing shape-controllable hydrogel microparticles with good monodispersity and unique morphology.In this review,we tried to provide an overview of the production of non-spherical microparticles composed of green hydrogel materials,emphasizing the microfluidic approaches.Furthermore,a brief introduction to their current applications is also presented.

关键词： Microfluidics Hydrogel Microparticles Non-spherical Anisotropic Green materials

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Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

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Green energy & Environment 2024年第3期9卷 544-555页

作者： Hengyuan Liu Xingjiang Wu Yuhao Geng Xin Li Jianhong Xu The State Key Laboratory of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

关键词： Iridium nanodots Carbon Microfluidic technology Efficient synthesis Electrocatalytic nitrogen fixation

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An efficient approach for the treatment of radioactive waste perfluoropolyether lubricants via a synergistic effect of thermal catalysis and immobilization

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Journal of Environmental Sciences 2024年第2期136卷 512-522页

作者： Xinhang Du Wenhua Tong Xinyu Zhou Jia Luo Yuqiu Liu Yabo Wang Panyu Li Yongkui Zhang department of Pharmaceutical&Biological engineering School of Chemical EngineeringSichuan UniversityChengdu 610065China

Perfluoropolyether(PFPE)lubricants are a kind of high-molecular polymer with many excellent properties.However,the use of PFPEs in the nuclear industry can lead to partial decomposition and carrying radionuclides,resulting in a large amount of radioactive waste PFPE lubricants annually.Moreover,radioactive waste PFPE lubricants are difficult to be effectively treated due to their high stability,the risk of possible leakage of radionuclides,and hypertoxic fluorine-containing by-products.In this study,without any precedent,a strategy of Mn O_(2)-catalyzed decomposition and Na_(2)CO_(3)-immobilized conversion was proposed for PFPE lubricant decomposition and fluorine immobilization simultaneously based on the Lewis acid-base and oxygen vacancies concept.A high fluorine conversion efficiency of 95.4%was achieved.Meanwhile,the mechanism of decomposition suggested that Mn O_(2)mainly provided Lewis acid sites and attacked the(basic)fluorine or oxygen atoms in PFPE molecules.The decomposition of PFPE chains was proceed down and volatile fluorine-containing gas was released by partial electron transfer,intramolecular disproportionation reaction,and unzipping fashion.Subsequently,gas by-products could be further oxidized and then immobilized into fluoride salts by carbonate solid absorbents.Overall,this study provides a simple,safe,and potentially practical strategy for the harmless conversion of refractory fluorinated organic wastes,especially perfluoropolymers.

关键词： Perfluoropolyether lubricants Catalyzed decomposition Fluorine-containing gas Immobilized conversion Fluoride

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Highly sensitive fluorescent sensing and photocatalytic degradation performance of two-dimensional Tb-organic network

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Journal of Rare Earths 2024年第2期42卷 303-313,I0003页

作者： Ting Gao Zhihu Ma Yixia Ren Zhixiang Wang Meili Zhang Xiaoli Chen Jijiang Wang Laboratory of New energy and New Function Materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'an716000China

A novel tetra-nuclear Tb-organic network,named as [Tb_(4)(2-pyia)_(6)(HAc)_(0.5)(2,2'-bipy)(H_(2)O)_(4.5)]·2,2'-bipy·H_(2)O(1),was synthesized hydrothermally based on 5-(pyridin-2-ylmethoxy) isophthalic acid(H_(2)pyia) and 2,2'-bipyridine(2,2'-bipy) ligands,and characterized by single crystal X-ray diffraction,thermogravimetric(TG) analyses,powder X-ray diffraction(PXRD) and infrared(IR) technology.1 possesses a two-dimensional network based on the tetra-nuclear inorganic building units,and the π-πstacking interactions between the pyia^(2-) ligands and the guest 2,2'-bipy molecules play an important role in the forming of 3D supramolecular structure.1 exhibits excellent fluorescent sensing performance for Fe^(3+)(1.26×10^(-8) mol/L),Cr_(2)O_(7)^(2-)(8.1×10^(-7) mol/L),2,4,6-trinitrophenol(TNP)(2.71×10^(-8) mol/L)and tetracycline(TCT)(2.76×10^(-7) mol/L) in aqueous solution with lower detection concentrations.The sensing mechanisms of 1 were investigated by density functional theory(DFT) calculations,ultraviolet-visible(UV-Vis) diffuse reflectance spectroscopy,PXRD and fluorescent lifetime analyses.The activated product of 1 was prepared by heating at 255℃ under constant pressure and used to photo-catalytically degrade TCT.Both 1 and the activated one have good photocatalytic degradation performance for TCT with degradation rates of 84.29% and 96.07%,respectively.The photocatalytic mechanisms were discovered by UV-Vis diffuse reflectance spectroscopy and radical trap experiments.The Tb-organic framework might be an excellent multifunctional fluorescent sensor and a good photocatalytic agent for TCT degradation in the future.

关键词： Tb-organic network Fluorescent sensing Photocatalytic degradation Rare earths

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Prediction of Ground State Configurations and Electrochemical Properties of Li_(3)InCl_(6) Doped with F, Br, and Ga

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Chinese Physics Letters 2024年第5期41卷 171-176页

作者：鲁征宇陈乐添胡绪陈素雅张旭周震 department of Materials Science and engineering Nankai UniversityTianjin 300350China Interdisciplinary Research Center for Sustainable energy Science and engineering School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001China

Compared with conventional solid-state electrolytes, halide solid-state electrolytes have several advantages such as a wider electrochemical window, better compatibility with oxide cathode materials, improved air stability,and easier preparation conditions making them conductive to industrial production. We concentrate on a typical halide solid-state electrolyte, Li_(3)InCl_(6), predict the most stable structure after doping with Br, F, and Ga by using the Alloy Theoretic Automated Toolkit based on first-principles calculations, and verify the accuracy of the prediction model. To investigate the potential of three equivalently doped ground state configurations of Li_(3)InCl_(6) as solid-state electrolytes for all-solid-state lithium-ion batteries, their specific properties such as crystal structure,band gap, convex packing energy, electrochemical stability window, and lithium-ion conductivity are computationally analyzed using first-principles calculations. After a comprehensive evaluation, it is determined that the F-doped ground state configuration Li_(3)InCl_(2.5)F_(3.5) exhibits better thermal stability, wider electrochemical stability window, and better lithium ion conductivity(1.80 m S·cm^(-1) at room temperature). Therefore, Li_(3)InCl_(2.5)F_(3.5) has the potential to be used in the field of all-solid-state lithium-ion batteries as a new type of halide electrolyte.

关键词： lithium stability electrolyte

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