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Adsorption behavior of CO2/H2S mixtures in calcite slit nanopores for CO2 storage:An insight from molecular perspective

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Petroleum Science 2024年第4期21卷 2444-2456页

作者： Cheng Qian Zhen-Hua Rui Yue-Liang Liu Kai Du Chen Liu Yang Zhao Xiao-Min Ma State Key Laboratory of Petroleum Resources and Engineering China University of Petroleum College of Petroleum Engineering China University of Petroleum College of Carbon Neutrality Future Technology China University of Petroleum College of Petroleum China University of Petroleum-Beijing at Karamay College of Mining Engineering Taiyuan University of Technology

It is acknowledged that injecting CO2into oil reservoirs and saline aquifers for storage is a practical and affordable method for *** CO2produced from industrial exhaust contains impurity gases such as H2S that might impact CO2sequestration due to competitive *** study makes a commendable effort to explore the adsorption behavior of CO2/H2S mixtures in calcite slit *** Canonical Monte Carlo（GCMC） simulation is employed to reveal the adsorption of CO2,H2S as well as their binary mixtures in calcite *** show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO2and H2S in calcite nanopores,***2exhibits stronger adsorption on calcite surface than *** energy plays the dominating role in the adsorption *** energy accounts for 97.11% of the CO2-calcite interaction energy and 56.33% of the H2S-calcite interaction energy at 10 MPa and 323.15 *** presence of H2S inhibits the CO2adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H2S leads to less *** quantity of CO2adsorbed is lessened by approximately 33% when the mole fraction of H2S reaches ***2molecules preferentially occupy the regions near the po re wall and H2S molecules tend to reside at the center of nanopore even when the molar ratio of CO2is low,indicating that CO2has an adsorption priority on the calcite surface over *** addition,moisture can weaken the adsorption of both CO2and H2S,while CO2is more *** interestingly,we find that pure CO2is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO2with H2S impurity should be settled in the deeper reservoirs.

关键词： Adsorption behavior CO 2 /H 2 S binary mixtures Molecular perspective Calcite slit nanopores CO 2 sequestration

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Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University The Institute of Green Chemistry and Engineering School of Chemistry and Chemical Engineering Nanjing University

The deep-processing utility of pure hydrogen sulfide （H2S） is a significant direction in natural gas chemical ***,a brand-new strategy of H2S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids （ILs） as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H2S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H2S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H2S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H 2 S conversion Catalysis

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Tourmaline guiding the electric field and dechlorination pathway of 2,3-dichlorophenol by Desulfitobacterium hafniense

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Journal of Environmental Sciences 2024年第1期135卷 262-273页

作者： Yue Lu Fangyi Liang Fanzhi Qin Linrui Zhong Jianhong Jiang Qi Liu Shoujuan Zhang Ming Yan Changzheng Fan Haoran Dong College of Environmental Science and Engineering Hunan UniversityChangsha 410082China Shenzhen Research Institute Hunan UniverisyShenzhen 510082China Key Laboratory of Environment Biology and Pollution Control Hunan UniversityMinistry of EducationChangsha 410082China China Machinery International Engineering Design&Research Institute Co. Ltd.Changsha 410007China Hunan Engineering Research Center for Water Treatment Process&Equipment Changsha 410007China

The dehalogenation of organohalides has been a research hotspot in bioremediation field;however,the influence of tourmaline,a natural ore that can generate spontaneous electric field,on organohalide-respiring bacteria(OHRB)and their dechlorination process is not well *** this study,the effect and mechanism of tourmaline on the reductive dechlorination of 2,3-dichlorophenol(2,3-DCP)by Desulfitobacterium hafniense DCB-2Twere *** characterization results confirmed that tourmaline had good stability and the optimal dosage of tourmaline was 2.5 g/L,which shortened the total time required for dechlorination reaction to 72 ***,tourmaline amendment also increased the proportion of 2-chlorophenol(2-CP)from 18%to 30%of end products,while that of 3-CP decreased *** theoretical calculations showed that the bond charge of the orthosubstituted chlorine declined from-0.179 to-0.067,and that of meta-substituted chlorine increased from-0.111 to-0.129,which indicated that the spontaneous electric field of tourmaline affected the charge distribution of 2,3-DCP and was more conducive to the generation of ***,tourmaline with the spontaneous electric field affected the reductive dechlorination pathway of Desulfitobacterium,and the tourmaline-OHRB combining system might serve as a novel strategy for the bioremediation of environments polluted with chlorinated phenols.

关键词： Reductive dechlorination Desulfitobacterium hafniense Tourmaline Electric field 2 3-dichlorophenol

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Exploring the impact of economic growth and energy consumption on SO2 emissions in China based on the Environmental Kuznets Curve hypothesis

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Petroleum Science 2024年第4期21卷 2892-2900页

作者： Bing-Jie Xu Yi-Fei Shen Hui Qiao Zhi Gao Faculty of Business City University of Macau Rural Development Institute Chinese Academy of Social Sciences School of Marxism Shenzhen Polytechnic University

This study aims to analysis the influence of economic growth(EG) and energy consumption(EC) on sulfur dioxide emissions(SE) in China. Accordingly, this study explores the link between EG, EC, and SE for 30 provinces in China over the span of 2000-2019. This study also analyzes cross-sectional dependence tests, panel unit root tests, Westerlund panel cointegration tests, Dumitrescu-Hurlin(D-H) causality tests. According to the test results, there is an inverted U-shaped association between EG and SE,and the assumption of the Environmental Kuznets Curve(EKC) is verified. The signs of EG and EC in the fixed effect(FE) and random effect(RE) methods are in line with those in the dynamic ordinary least squares(DOLS), fully modified ordinary least squares(FMOLS) and autoregressive distributed lag(ARDL)estimators. Moreover, the results verified that EC can obviously positive impact the SE. To reduce SE in China, government and policymakers can improve air quality by developing cleaner energy sources and improving energy efficiency. This requires the comprehensive use of policies, regulations, economic incentives, and public participation to promote sustainable development.

关键词： SO 2 emissions Economic growth Energy consumption EKC China

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Performance and enhanced oil recovery efficiency of an acid-resistant polymer microspheres of anti-CO2 channeling in low-permeability reservoirs

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Petroleum Science 2024年第4期21卷 2420-2432页

作者： Hai-Zhuang Jiang Hong-Bin Yang Ruo-Sheng Pan Zhen-Yu Ren Wan-Li Kang Jun-Yi Zhang Shi-Long Pan Bauyrzhan Sarsenbekuly State Key Laboratory of Deep Oil and Gas China University of Petroleum (East China) School of Petroleum Engineering China University of Petroleum (East China) Oil and Gas Engineering Research Institute School of Energy and Petroleum Industry Kazakh-British Technical University

CO2flooding is a vital development method for enhanced oil recovery in low-permeability reservoirs,However,micro-fractures are developed in low-permeability reservoirs,which are essential oil flow channels but can also cause severe CO2gas channeling ***,anti-gas channeling is a necessary measure to improve the effect of *** kind of anti-gas channeling refers to the plugging of fractures in the deep formation to prevent CO2gas channeling,which is different from the wellbore *** microspheres have the characteristics of controllable deep plugging,which can achieve the profile control of low-permeability fractured *** acidic environments with supercritical CO2,traditional polymer microspheres have poor expandability and plugging *** on previous work,a systematic evaluation of the expansion performance,dispersion rheological properties,stability,deep migration,anti-CO2channeling and enhanced oil recovery ability of a novel acid-resistant polymer microsphere（DCNPM-A） was carried out under CQ oilifield conditions（salinity of85,000 mg/L,80℃,pH=3）.The results show that the DCNPM-A microsphere had a better expansion performance than the traditional microsphere,with a swelling rate of *** microsphere dispersion with a concentration of 0.1%-0.5% had the advantages of low viscosity,high dispersion and good injectability in the low permeability fractured *** the acidic environment of supercritical CO2,DCNPM-A microspheres showed excellent stability and could maintain strength for over 60 d with less *** core experiments,DCNPM-A microspheres exhibited delayed swelling characteristics and could effectively plug deep *** a plugging rate of 95%,the subsequent enhanced oil recovery of CO2flooding could reach 21.03%.The experimental results can provide a theoretical basis for anti-CO2channeling and enhanced oil recovery in low-permeability fractured reservoirs.

关键词： Low-permeability reservoir Anti-CO 2 channeling Polymer microsphere Acid resistance

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Nitrogen-doping boosts *CO utilization and H2O activation on copper for improving CO2 reduction to C2+ products

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Green Energy & Environment 2024年第9期9卷 1459-1465页

作者： Yisen Yang Zhonghao Tan Jianling Zhang Jie Yang Renjie Zhang Sha Wang Yi Song Zhuizhui Su Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences School of Chemical Sciences University of Chinese Academy of Sciences Key Laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences

To improve the electrocatalytic transformation of carbon dioxide （CO2） to multi-carbon (C2+) products is of great *** we developed a nitrogen-doped Cu catalyst,by which the maximum C2+Faradaic efficiency can reach 72.7%in flow-cell system,with the partial current density reaching 0.62 A *** in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst,thus promoting the*CO utilization in the subsequent C–C coupling ***,the water activation can be well enhanced by N doping on Cu *** to the synergistic effects,the selectivity and activity for C2+products over the N-deoped Cu catalyst are much improved.

关键词： Electrocatalytic CO 2 reduction reaction Copper catalyst Doping Multi-carbon products In situ Raman measurement

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Transforming liquid flow fuel cells to controllable reactors for highlyefficient oxidation of 5-hydroxymethylfurfural to 2, 5-furandicarboxylic acid at low temperature

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Journal of Energy Chemistry 2024年第3期90卷 621-631,I0014页

作者： Ye Qiang Xi Liu Denghao Ouyang Zhao Jiang Xuebing Zhao Key Laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Institute of Applied Chemistry Department of Chemical EngineeringTsinghua UniversityBeijing 100084China School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'an 710049ShaanxiChina

Highly-efficient oxidation of 5-hydroxymethylfurtural(HMF) to 2,5-furandicarboxylic acid(FDCA) at low temperature with air as the oxidant is still ***,inspired by the respirato ry electron transport chain(ETC) of living cells mediated by electron carriers,we constructed artificial ETCs and transformed liquid flow fuel cells(LFFCs) to flexible reactors for efficient oxidation of HMF to produce FDCA under mild *** LFFC reactor employed an electrodeposition modified nickel foam as an anode to promote HMF oxidation and(VO_(2))_(2)SO_(4) as a cathode electron carrier to facilitate the electron transfer to *** reaction rate could be easily controlled by selecting the anode catalyst,adjusting the external loading and changing the cathodic electron carrier or oxidants.A maximal power density of 44.9 mW cm^(-2) at room temperature was achieved,while for FDCA production,short-circuit condition was preferred to achieve quick transfer of *** a single batch operation with 0.1 M initial HMF,FDCA yield reached 97.1%.By fed-batch operation,FDCA concentration reached 144.5 g L^(-1) with a total yield of 96%.Ni^(2+)/Ni^(3+) redox couple was the active species mediating the electron transfer,while both experimental and DFT calculation results indicated that HMFCA pathway was the preferred reaction mechanism.

关键词： 5-Hydroxymethylfurfural 2 5-Furandicarboxylic acid Electrodeposition Electron transport chain Liquid flow fuel cell

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Homovalent doping: An efficient strategy of the enhanced TiNb2O7 anode for lithium-ion batteries

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Green Energy & Environment 2024年第8期9卷 1257-1266页

作者： Xiaohe Jin Yirui Deng Han Tian Miaomiao Zhou Wenhao Tang Huiyou Dong Xinquan Zhang Ruiping Liu Department of Materials Science and Engineering China University of Mining & Technology (Beijing) Department of Materials Science and Engineering China University of Mining&Technology (Beijing)

The low energy density,unsatisfied cycling performance,potential safety issue and slow charging kinetics of the commercial lithium-ion batteries restrained their further application in the fields of fast charging and long-haul electric *** TiNb2O7（TNO） with the theoretical capacity of 387 mAh g-1has been proposed as a high-capacity anode materials to replace *** this work,homovalent doping strategy was used to enhance the electrochemical performance of Ti Nb2O7（TNO） by employing Zr to partial substitute Ti through solvothermal *** doping of Zr4+ions can enlarge the lattice structure without changing the chemical valence of the original elements,refine and homogenize the grains,improve the electrical conductivity,and accelerate the ion diffusion kinetics,and finally enhance the cycle and rate ***,Z0.05-TNO shows initial discharge capacity of as high as 312.2 mAh g-1at 1 C and 244.8 mAh g-1at 10 C,and still maintains a high specific capacity of 171.3 mAh g-1after 800 cycles at 10 *** study provides a new strategy for high-performance fastcharging energy storage electrodes.

关键词： Homovalent doping Zr 4+ TiNb 2 O 7 Microsphere Lithium-ion batteries

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Oxygen-vacancy-rich MnO_(x)supported RuO_(x)for efficient base-free oxidation of 5-hydroxymethylfurfural and 5-methoxymethylfurfural to 2,5-furandicarboxylic acid

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Journal of Energy Chemistry 2024年第8期95卷 670-683,I0015页

作者： Jiali Wu Weizhen Xie Yining Zhang Xixian Ke Tianyuan Li Huayu Fang Yong Sun Xianhai Zeng Lu Lin Xing Tang Xiamen Key Laboratory of Clean and High-valued Applications for Biomass Fujian Engineering and Research Center of Clean and High-valued Technologies for BiomassCollege of EnergyXiamen UniversityXiamen 361102FujianChina Key Lab for Sport Shoes Upper Materials of Fujian Province Fujian Engineering and Research Center for New Functional Fiber Materials(Fujian Huafeng New Material Co.Ltd.Putian Dakai New Material Co.Ltd.)Putian 351144FujianChina

2,5-Furandicarboxylic acid(FDCA)is a promising biomass-derived polymeric monomer that serves as an attractive alternative to terephthalic acid derived from fossil ***,the green and efficient production of FDCA through the oxidation of 5-hydroxymethylfurfural(HMF)and its derivatives is still rudimentary under base-free *** this work,oxygen-vacancy-rich Mn Oxwas prepared and displayed a strong adsorption and anchoring ability to Ru species that mainly exposed the(210)plane of RuO_(2),bringing about highly dispersed and active interfacial Ru-O-Mn *** results and density functional theory calculations confirm that these above features greatly facilitate the adsorption/activation of oxygen and the dehydrogenation-oxidation of HMF/5-methoxymethylfurfural(MMF),which enables an efficient FDCA production under base-free and mild ***,a desirable FDCA yield of 86.56%was still obtained from concentrated HMF(10 wt%)under base-free conditions over oxygen-vacancy-rich Mn Oxsupported Ru Ox(1.0 MPaO_(2),120℃,6 h).This work delineates a facile catalyst preparation strategy for HMF/MMF oxidation,and might open a new avenue for the green synthesis of FDCA under base-free conditions.

关键词： Base-free oxidation Oxygen-vacancy-rich 5-Hydroxymethylfurfural 5-Methoxymethylfurfural 2 5-Furandicarboxylic acid

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Cell-free biocatalysis coupled with photo-catalysis and electro-catalysis: Efficient CO2-to-chemical conversion

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Green Energy & Environment 2024年第9期9卷 1366-1383页

作者： Junzhu Yang Chi-Kit Sou Yuan Lu Key Laboratory of Industrial Biocatalysis Ministry of Education Tsinghua University Department of Chemical Engineering Tsinghua University

The increasing atmospheric carbon dioxide （CO2） concentration has exposed a series of crises in the earth's ecological *** to effectively fix and convert carbon dioxide into products with added value has attracted the attention of many ***-free enzyme catalytic system coupled with electrical and light have been a promising attempt in the field of biological carbon fixation in recent *** this review,the research progresses of photoenzyme catalysis,electroenzyme catalysis and photo-electroenzyme catalysis for converting carbon dioxide into chemical products in cell-free systems are systematically *** focus on reviewing and comparing various coupling methods and principles of photoenzyme catalysis and electroenzyme catalysis in cell-free systems,especially the materials used in the construction of the coupling system,and analyze and point out the characteristics and possible problems of different coupling ***,we discuss the major challenges and prospects of coupling physical signals and cell-free enzymatic catalytic systems in the field of CO2fixation,suggesting possible strategies to improve the carbon sequestration capacity of such systems.

关键词： CO 2 fixation Cell-free system Enzyme Photoenzyme catalysis Electroenzyme catalysis

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