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Gas-phase electrocatalytic reduction of carbon dioxide using electrolytic cell based on phosphoric acid-doped polybenzimidazole membrane 被引量:3
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作者 Dunfeng Gao Fan Cai +3 位作者 Qinqin Xu Guoxiong Wang Xiulian Pan Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第6期694-700,共7页
Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an el... Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an electrolytic cell, constructed using phosphoric acid-doped polybenz- imidazole (PBI) membrane, which allowed operation at 170 ℃ Pt/C and PtMo/C with variable ratio of Pt/Mo were studied as the cathode catalysts. The results showed that PtMo/C catalysts significantly enhanced CO formation and inhibited CH4 formation compared with Pt/C catalyst. Characterization by X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy revealed that most Mo species existed as MoO3 in PtMo/C catalysts and the interaction between Pt and MoOx was likely responsible for the enhanced CO formation rate although these bicomponent catalysts in general had a larger particle size than Pt/C catalyst. 展开更多
关键词 carbon dioxide gas-phase electrocatalytic reduction platinum-molybdenum catalyst Faradaic efficiency formation rate
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Efficient electrocatalytic reduction of carbon dioxide to ethylene on copper–antimony bimetallic alloy catalyst 被引量:6
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作者 Shuaiqiang Jia Qinggong Zhu +6 位作者 Haihong Wu Meng’en Chu Shitao Han Ruting Feng Jinghui Tu Jianxin Zhai Buxing Han 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第7期1091-1098,共8页
The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 red... The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 reduction.In this work,we synthesize a series of porous bimetallic Cu–Sb alloys with different compositions for the catalytic reduction of CO2 to C2H4.It is demonstrated that the alloy catalysts are much more efficient than the pure Cu catalyst.The performance of the alloy catalysts depended strongly on the composition.Further,the alloy with a Cu:Sb ratio of 10:1 yielded the best results;it exhibited a high C2H4 Faradaic efficiency of 49.7%and a high current density of 28.5 mA cm?2 at?1.19 V vs.a reversible hydrogen electrode(RHE)in 0.1 M KCl solution.To the best of our knowledge,the electrocatalytic reduction of CO2 to C2H4 using Cu–Sb alloys as catalysts has not been reported.The excellent performance of the porous alloy catalyst is attributed to its favorable electronic configuration,large surface area,high CO2 adsorption rate,and fast charge transfer rate. 展开更多
关键词 carbon dioxide reduction Ethyene ELECTROCATALYST Copper-antimony bimetallic alloy Synergistic effect
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A perspective on the electrocatalytic conversion of carbon dioxide to methanol with metallomacrocyclic catalysts 被引量:6
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作者 Xinyan Liu Bo-Quan Li +2 位作者 Bing Ni Lei Wang Hong-Jie Peng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第1期263-275,I0008,共14页
Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy supply.Methanol ... Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy supply.Methanol is an ideal energy carrier as alternative fuels and one of the most important commodity chemicals.Nevertheless,methanol is currently mainly produced from fossil-based syngas,the production of which yields tremendous carb on emission globally.Direct CO_(2)R towards metha nol poses great potential to shift the paradigm of methanol production.In this perspective,we focus our discussions on producing methanol from electrochemical CO_(2)R,using metallomacrocyclic molecules as the model catalysts.We discuss the motivation of having methanol as the sole CO_(2)R product,the documented application of metallomacrocyclic catalysts for CO_(2)R,and recent advance in catalyzing CO_(2) to methanol with cobalt phthalocyanine-based catalysts.We attempt to understand the key factors in determining the activity,selectivity,and stability of electrocatalytic CO_(2)-to-methanol conversion,and to draw mechanistic insights from existing observations.Finally,we identify the challenges hindering methanol electrosynthesis directly from CO_(2) and some intriguing directions worthy of further investigation and exploration. 展开更多
关键词 carbon dioxide reduction METHANOL ELECTROCATALYSIS Molecular catalysts Single atom catalysts HETEROGENIZATION
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Cascade electrocatalytic reduction of carbon dioxide and nitrate to ethylamine 被引量:4
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作者 Zixu Tao Yueshen Wu +3 位作者 Zishan Wu Bo Shang Conor Rooney Hailiang Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第2期367-370,共4页
CO_(2) utilization,including electrochemical reduction of CO_(2) to fuels and useful chemicals,is explored to valorize carbon emissions[1–12].The value of CO_(2) electroreduction products originates from their C–H,C... CO_(2) utilization,including electrochemical reduction of CO_(2) to fuels and useful chemicals,is explored to valorize carbon emissions[1–12].The value of CO_(2) electroreduction products originates from their C–H,C–C,and C–O bonds.To further increase the value and expand the scope of products,it is desirable to integrate C–N bond formation with the electrochemical reduction of CO_(2). 展开更多
关键词 NITRATE dioxide carbon
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Operando Converting BiOCl into Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) for Efficient Electrocatalytic Reduction of Carbon Dioxide to Formate 被引量:2
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作者 Huai Qin Fu Junxian Liu +10 位作者 Nicholas M.Bedford Yun Wang Joshua Wright Peng Fei Liu Chun Fang Wen Liang Wang Huajie Yin Dongchen Qi Porun Liu Hua Gui Yang Huijun Zhao 《Nano-Micro Letters》 SCIE EI CAS CSCD 2022年第7期263-278,共16页
Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismu... Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismuth oxides and subcarbonate encounter stability issues. This work is designated to exemplify that the operando synthesis can be an effective means to enhance the stability of electrocatalysts under operando CO_(2)RR conditions. A synthetic approach is developed to electrochemically convert Bi^(O)Cl into Cl-containing subcarbonate(Bi_(2)O_(2)(CO_(3))_(x)Cl_(y)) under operando CO_(2)RR conditions. The systematic operando spectroscopic studies depict that BiOCl is converted to Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) via a cathodic potential-promoted anion-exchange process. The operando synthesizedBi_(2)O_(2)(CO_(3))_(x)Cl_(y) can tolerate-1.0 V versus RHE, while for the wet-chemistry synthesized pure Bi_(2)O_(2)CO_(3),the formation of metallic Bio occurs at-0.6 V versus RHE. At-0.8 V versus RHE, Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) can readily attain a FEHCOO-of 97.9%,much higher than that of the pure Bi_(2)O_(2)CO_(3)(81.3%). DFT calculations indicate that differing from the pure Bi_(2)O_(2)CO_(3)-catalyzed CO_(2)RR, where formate is formed via a *OCHO intermediate step that requires a high energy input energy of 2.69 eV to proceed, the formation of H COO-over Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) has proceeded via a *COOH intermediate step that only requires low energy input of 2.56 eV. 展开更多
关键词 carbon dioxide reduction Chloride-containing bismuth subcarbonate Cathodic potential-promoted anion-exchange Stability
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Structural and interfacial engineering of well‐defined metal‐organic ensembles for electrocatalytic carbon dioxide reduction
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作者 Fenglei Lyu Wei Hua +3 位作者 Huirong Wu Hao Sun Zhao Deng Yang Peng 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第6期1417-1432,共16页
Electrochemical carbon dioxide reduction(CO_(2)RR)has been generally regarded as green technologies that can convert renewable energy such as sunlight and wind into fuels and valuable chemicals.However,the large‐scal... Electrochemical carbon dioxide reduction(CO_(2)RR)has been generally regarded as green technologies that can convert renewable energy such as sunlight and wind into fuels and valuable chemicals.However,the large‐scale implementation of CO_(2)RR is severely hindered by the lack of high‐performance CO_(2)RR electrocatalysts.Heterogeneous molecular catalysts and metal‐organic framework with well‐defined structure and high tunability of the metal centers and ligands show great promise for CO_(2)RR in terms of both fundamental understanding and practical application.Here,structural and interfacial engineering of these well‐defined metal‐organic ensembles is summarized.This review starts from the fundamental electrochemistry of CO_(2)RR and its evaluation criteria,and then moves to the heterogeneous molecular catalysts and metal‐organic framework with emphasis on the engineering of metal centers and ligands,their interaction with supports,as well as in situ reconstruction of metal‐organic ensembles.Summary and outlook are present in the end,with the hope to inspire and provoke more genuine thinking on the design and fabrication of efficient CO_(2)RR electrocatalysts. 展开更多
关键词 carbon dioxide reduction ELECTROCATALYSIS Heterogeneous molecular catalyst Metal‐organic frameworks In situ reconstruction
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Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation 被引量:1
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作者 Hengyuan Liu Xingjiang Wu +2 位作者 Yuhao Geng Xin Li Jianhong Xu 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第3期544-555,共12页
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-... 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. 展开更多
关键词 Iridium nanodots carbon Microfluidic technology Efficient synthesis electrocatalytic nitrogen fixation
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Chemico-biological conversion of carbon dioxide 被引量:1
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作者 Liangwei Hu Junzhu Yang +3 位作者 Qi Xia Jin Zhang Hongxin Zhao Yuan Lu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第2期371-387,I0009,共18页
The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challen... The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges. 展开更多
关键词 carbon dioxide Bioelectric synthesis Artificial photosynthesis Synthetic product
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Effects of drip and flood irrigation on carbon dioxide exchange and crop growth in the maize ecosystem in the Hetao Irrigation District,China 被引量:1
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作者 LI Chaoqun HAN Wenting PENG Manman 《Journal of Arid Land》 SCIE CSCD 2024年第2期282-297,共16页
Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation metho... Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation methods on carbon dioxide(CO_(2))exchange and crop growth in this region.The experimental site was divided into drip and flood irrigation zones.The irrigation schedules of this study aligned with the local commonly used irrigation schedule.We employed a developed chamber system to measure the diurnal CO_(2)exchange of maize plants during various growth stages under both drip and flood irrigation methods.From May to September in 2020 and 2021,two sets of repeated experiments were conducted.In each experiment,a total of nine measurements of CO_(2)exchange were performed to obtain carbon exchange data at different growth stages of maize crop.During each CO_(2)exchange measurement event,CO_(2)flux data were collected every two hours over a day-long period to capture the diurnal variations in CO_(2)exchange.During each CO_(2)exchange measurement event,the biological parameters(aboveground biomass and crop growth rate)of maize and environmental parameters(including air humidity,air temperature,precipitation,soil water content,and photosynthetically active radiation)were measured.The results indicated a V-shaped trend in net ecosystem CO_(2)exchange in daytime,reducing slowly at night,while the net assimilation rate(net primary productivity)exhibited a contrasting trend.Notably,compared with flood irrigation,drip irrigation demonstrated significantly higher average daily soil CO_(2)emission and greater average daily CO_(2)absorption by maize plants.Consequently,within the maize ecosystem,drip irrigation appeared more conducive to absorbing atmospheric CO_(2).Furthermore,drip irrigation demonstrated a faster crop growth rate and increased aboveground biomass compared with flood irrigation.A strong linear relationship existed between leaf area index and light utilization efficiency,irrespective of the irrigation method.Notably,drip irrigation displayed superior light use efficiency compared with flood irrigation.The final yield results corroborated these findings,indicating that drip irrigation yielded higher harvest index and overall yield than flood irrigation.The results of this study provide a basis for the selection of optimal irrigation methods commonly used in the Hetao Irrigation District.This research also serves as a reference for future irrigation studies that consider measurements of both carbon emissions and yield simultaneously. 展开更多
关键词 carbon dioxide exchange maize growth drip irrigation harvest index net primary productivity Hetao Irrigation District
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Carbon dioxide enrichment affected flower numbers transiently and increased successful post-pollination development stably but without altering final acorn production in mature pedunculate oak (Quercus robur L.)
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作者 Ryan McClory Richard H.Ellis +5 位作者 Martin Lukac Jo Clark Carolina Mayoral Kris M.Hart Andrew R.G.Plackett A.Rob MacKenzie 《Journal of Forestry Research》 SCIE EI CAS CSCD 2024年第4期1-12,共12页
Acorn production in oak(Quercus spp.)shows considerable inter-annual variation,known as masting,which provides a natural defence against seed predators but a highly-variable supply of acorns for uses such as in commer... Acorn production in oak(Quercus spp.)shows considerable inter-annual variation,known as masting,which provides a natural defence against seed predators but a highly-variable supply of acorns for uses such as in commercial tree planting each year.Anthropogenic emissions of greenhouse gases have been very widely reported to influence plant growth and seed or fruit size and quantity via the‘fertilisation effect’that leads to enhanced photosynthesis.To examine if acorn production in mature woodland communities will be affected by further increase in CO_(2),the contents of litter traps from a Free Air Carbon Enrichment(FACE)experiment in deciduous woodland in central England were analysed for numbers of flowers and acorns of pedunculate oak(Quercus robur L.)at different stages of development and their predation levels under ambient and elevated CO_(2) concentrations.Inter-annual variation in acorn numbers was considerable and cyclical between 2015 and 2021,with the greatest numbers of mature acorns in 2015,2017 and 2020 but almost none in 2018.The numbers of flowers,enlarged cups,immature acorns,empty acorn cups,and galls in the litter traps also varied amongst years;comparatively high numbers of enlarged cups were recorded in 2018,suggesting Q.robur at this site is a fruit maturation masting species(i.e.,the extent of abortion of pollinated flowers during acorn development affects mature acorn numbers greatly).Raising the atmospheric CO_(2) concentration by 150μL L^(−1),from early 2017,increased the numbers of immature acorns,and all acorn evidence(empty cups+immature acorns+mature acorns)detected in the litter traps compared to ambient controls by 2021,but did not consistently affect the numbers of flowers,enlarged cups,empty cups,or mature acorns.The number of flowers in the elevated CO_(2) plots’litter traps was greater in 2018 than 2017,one year after CO_(2) enrichment began,whereas numbers declined in ambient plots.Enrichment with CO_(2) also increased the number of oak knopper galls(Andricus quercuscalicis Burgsdorf).We conclude that elevated CO_(2) increased the occurrence of acorns developing from flowers,but the putative benefit to mature acorn numbers may have been hidden by excessive pre-and/or post-dispersal predation.There was no evidence that elevated CO_(2) altered masting behaviour. 展开更多
关键词 Quercus robur L. ACORNS MASTING Pedunculate oak carbon dioxide
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CAS-ESM2.0 Dataset for the Carbon Dioxide Removal Model Intercomparison Project(CDRMIP)
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作者 Jiangbo JIN Duoying JI +9 位作者 Xiao DONG Kece FEI Run GUO Juanxiong HE Yi YU Zhaoyang CHAI He ZHANG Dongling ZHANG Kangjun CHEN Qingcun ZENG 《Advances in Atmospheric Sciences》 SCIE CAS CSCD 2024年第5期989-1000,共12页
Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation stra... Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation strategies in the near future.In this study,we generate a dataset by conducting an experiment involving carbon dioxide removal(CDR)—a potential way to suppress global warming—using the Chinese Academy of Sciences Earth System Model version 2.0(CASESM2.0).A preliminary evaluation is provided.The model is integrated from 200–340 years as a 1%yr^(−1) CO_(2) concentration increase experiment,and then to~478 years as a carbon dioxide removal experiment until CO_(2) returns to its original value.Finally,another 80 years is integrated in which CO_(2) is kept constant.Changes in the 2-m temperature,precipitation,sea surface temperature,ocean temperature,Atlantic meridional overturning circulation(AMOC),and sea surface height are all analyzed.In the ramp-up period,the global mean 2-m temperature and precipitation both increase while the AMOC weakens.Values of all the above variables change in the opposite direction in the ramp-down period,with a delayed peak relative to the CO_(2) peak.After CO_(2) returns to its original value,the global mean 2-m temperature is still~1 K higher than in the original state,and precipitation is~0.07 mm d^(–1) higher.At the end of the simulation,there is a~0.5°C increase in ocean temperature and a 1 Sv weakening of the AMOC.Our model simulation produces similar results to those of comparable experiments previously reported in the literature. 展开更多
关键词 CAS-ESM2.0 CDRMIP carbon dioxide removal AMOC temperature PRECIPITATION sea surface height
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Simultaneous Degradation, Dehalogenation, and Detoxification of Halogenated Antibiotics by Carbon Dioxide Radical Anions
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作者 Yanzhou Ding Xia Yu +8 位作者 Shuguang Lyu Huajun Zhen Wentao Zhao Cheng Peng Jiaxi Wang Yiwen Zhu Chengfei Zhu Lei Zhou Qian Sui 《Engineering》 SCIE EI CAS CSCD 2024年第6期78-86,共9页
Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number ... Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment. 展开更多
关键词 carbon dioxide radical anions Advanced reduction processes Halogenated antibiotics DEHALOGENATION DETOXIFICATION
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Accelerating H^(*)desorption of hollow Mo_(2)C nanoreactor via in-situ grown carbon dots for electrocatalytic hydrogen evolution
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作者 Mengmeng Liu Yuanyuan Jiang +3 位作者 Zhuwei Cao Lulu Liu Hong Chen Sheng Ye 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期464-471,共8页
Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improv... Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds. 展开更多
关键词 Mo_(2)C nanoreactor carbon dots H^(*)desorption electrocatalytic hydrogen evolution
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Experimental investigation on pyrolysis products and pore structure characteristics of organic-rich shale heated by supercritical carbon dioxide
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作者 Bai-Shuo Liu Chuan-Jin Yao +3 位作者 Jia-Long Qi Ya-Qian Liu Liang Xu Jing-Xuan Hou 《Petroleum Science》 SCIE EI CAS CSCD 2024年第4期2393-2406,共14页
The efficient pyrolysis and conversion of organic matter in organic-rich shale,as well as the effective recovery of pyrolysis shale oil and gas,play a vital role in alleviating energy pressure.The state of carbon diox... The efficient pyrolysis and conversion of organic matter in organic-rich shale,as well as the effective recovery of pyrolysis shale oil and gas,play a vital role in alleviating energy pressure.The state of carbon dioxide(CO_(2))in the pyrolysis environment of shale reservoirs is the supercritical state.Its unique supercritical fluid properties not only effectively heat organic matter,displace pyrolysis products and change shale pore structure,but also achieve carbon storage to a certain extent.Shale samples were made into powder and three sizes of cores,and nitrogen(N_(2))and supercritical carbon dioxide(ScCO_(2))pyrolysis experiments were performed at different final pyrolysis temperatures.The properties and mineral characteristics of the pyrolysis products were studied based on gas chromatography analysis,Xray diffraction tests,and mass spectrometry analysis.Besides,the pore structure characteristics at different regions of cores before and after pyrolysis were analyzed using N_(2) adsorption tests to clarify the impact of fracturing degree on the pyrolysis effect.The results indicate that the optimal pyrolysis temperature of Longkou shale is about 430℃.Compared with N_(2),the oil yield of ScCO_(2) pyrolysis is higher.The pyrolysis oil obtained by ScCO_(2) extraction has more intermediate fractions and higher relative molecular weight.The ScCO_(2) can effectively improve the pore diameter of shale and its effect is better than that of N_(2).The micropores are produced in shale after pyrolysis,and the macropores only are generated in ScCO_(2) pyrolysis environments with temperatures greater than 430℃.The pore structure has different development characteristics at different pyrolysis temperatures,which are mainly affected by the pressure holding of volatile matter and products blocking.Compared to the surface of the core,the pore development effect inside the core is better.With the decrease in core size,the pore diameter,specific surface area,and pore volume of cores all increase after pyrolysis. 展开更多
关键词 Organic-rich shale Supercritical carbon dioxide In-situ pyrolysis Pore structure Core size and region
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The AVO Effect of Formation Pressure on Time-Lapse Seismic Monitoring in Marine Carbon Dioxide Storage
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作者 Fan Wu Qingping Li +1 位作者 Yufa He Jingye Li 《哈尔滨工程大学学报(英文版)》 CSCD 2024年第3期645-655,共11页
The phase change of CO_(2) has a significant bearing on the siting, injection, and monitoring of storage. The phase state of CO_(2) is closely related to pressure. In the process of seismic exploration, the informatio... The phase change of CO_(2) has a significant bearing on the siting, injection, and monitoring of storage. The phase state of CO_(2) is closely related to pressure. In the process of seismic exploration, the information of formation pressure can be response in the seismic data. Therefore, it is possible to monitor the formation pressure using time-lapse seismic method. Apart from formation pressure, the information of porosity and CO_(2) saturation can be reflected in the seismic data. Here, based on the actual situation of the work area, a rockphysical model is proposed to address the feasibility of time-lapse seismic monitoring during CO_(2) storage in the anisotropic formation. The model takes into account the formation pressure, variety minerals composition, fracture, fluid inhomogeneous distribution, and anisotropy caused by horizontal layering of rock layers(or oriented alignment of minerals). From the proposed rockphysical model and the well-logging, cores and geological data at the target layer, the variation of P-wave and S-wave velocity with formation pressure after CO_(2) injection is calculated. And so are the effects of porosity and CO_(2) saturation. Finally, from anisotropic exact reflection coefficient equation, the reflection coefficients under different formation pressures are calculated. It is proved that the reflection coefficient varies with pressure. Compared with CO_(2) saturation, the pressure has a greater effect on the reflection coefficient. Through the convolution model, the seismic record is calculated. The seismic record shows the difference with different formation pressure. At present, in the marine CO_(2) sequestration monitoring domain, there is no study involving the effect of formation pressure changes on seismic records in seafloor anisotropic formation. This study can provide a basis for the inversion of reservoir parameters in anisotropic seafloor CO_(2) reservoirs. 展开更多
关键词 Time-lapse seismic monitoring Marine carbon dioxide storage AVO modeling Formation pressure Anisotropic Rockphysical model
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Solubility of iron(Ⅲ) and nickel(Ⅱ) acetylacetonates in supercritical carbon dioxide
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作者 Haixin Sun Jianlei Qi +4 位作者 Jianfei Sun Lin Li Kunpeng Yu Jintao Wu Jianzhong Yin 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第1期29-34,共6页
As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates hav... As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range. 展开更多
关键词 Iron(III)acetylacetonate Nickel(II)acetylacetonate Supercritical carbon dioxide Solubility measurement Correlation model Phase equilibrium
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Simulation Modelling and Techno-Economics of Supercritical Carbon Dioxide Recompression Closed Brayton Cycle
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作者 Ken Amaale Atinga 《Energy and Power Engineering》 2024年第10期325-344,共20页
In recent years, there has been global interest in meeting targets relating to energy affordability and security while taking into account greenhouse gas emissions. This has heightened major interest in potential inve... In recent years, there has been global interest in meeting targets relating to energy affordability and security while taking into account greenhouse gas emissions. This has heightened major interest in potential investigations into the use of supercritical carbon dioxide (sCO2) power cycles. Climate change mitigation is the ultimate driver for this increased interest;other relevant issues include the potential for high cycle efficiency and a circular economy. In this study, a 25 MWe recompression closed Brayton cycle (RCBC) has been assessed, and sCO2 has been proposed as the working fluid for the power plant. The methodology used in this research work comprises thermodynamic and techno-economic analysis for the prospective commercialization of this sCO2 power cycle. An evaluated estimation of capital expenditure, operational expenditure, and cost of electricity has been considered in this study. The ASPEN Plus simulation results have been compared with theoretical and mathematical calculations to assess the performance of the compressors, turbine, and heat exchangers. The results thus reveal that the cycle efficiency for this prospective sCO2 recompression closed Brayton cycle increases (39% - 53.6%) as the temperature progressively increases from 550˚C to 900˚C. Data from the Aspen simulation model was used to aid the cost function calculations to estimate the total capital investment cost of the plant. Also, the techno-economic results have shown less cost for purchasing equipment due to fewer components being required for the cycle configuration as compared to the conventional steam power plant. 展开更多
关键词 Supercritical carbon dioxide (sCO2) Closed Brayton Cycle TECHNO-ECONOMICS Simulation Capital Expenditure Gas Turbine THERMODYNAMIC Equipment Cost Optimization and Sensitivity
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Optimization of Supercritical Carbon dioxide Extraction of Ginger Essential Oil by Response Surface Method 被引量:5
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作者 雷红 周仁杰 +2 位作者 魏巧年 李晓乐 吴静 《Agricultural Science & Technology》 CAS 2016年第9期2178-2182,共5页
[Objective] Ginger essential oil (GEO) is widely used in food production and medical field in recent years due to its prominent biological functions, and this study was conducted to obtain high-quality and high-puri... [Objective] Ginger essential oil (GEO) is widely used in food production and medical field in recent years due to its prominent biological functions, and this study was conducted to obtain high-quality and high-purity ginger essential oil from the fresh ginger. [Method] GEO was extracted from ginger roots by supercritical fluid extraction (SFE) method. The effects of flow rate of CO2, mesh size of ginger powder and volume of entrainer were investigated by single-factor experiments and response surface method. The content and extraction rate of 6-gingerol represented the extraction index of GEO. [Result] The conditions were optimized as follows: flow rate of CO2 at 25 L/h, mesh size of ginger power of 80 mesh, and volume of anhydrous ethanol as entrainer of 92.46 ml. The optimal extraction rate of 6-gingerol was 3.21%, which was predicted by RSM. [Conclusion] The optimal process of supercritical carbon dioxide extraction of ginger essential oil was identified by singlefactor experiments and response surface method. The present study provides a satisfactory method for purifying GEO from ginger for industrial purpose. 展开更多
关键词 Ginger essential oil (GEO) Supercritical carbon dioxide extraction Response surface methodology
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Vapor-Liquid Equilibrium Data of Carbon Dioxide+Methyl Propionate and Carbon Dioxide+Propyl Propionate Systems
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作者 徐伟 谢传欣 +1 位作者 李洪玲 田宜灵 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2010年第3期317-324,I0002,共9页
High-pressure vapor-liquid equilibrium data for the binary systems of methyl propionate+carbon dioxide and propyl propionate+carbon dioxide were measured at pressure from 1.00 MPa to 12.00 MPa and temperature in the... High-pressure vapor-liquid equilibrium data for the binary systems of methyl propionate+carbon dioxide and propyl propionate+carbon dioxide were measured at pressure from 1.00 MPa to 12.00 MPa and temperature in the range from 313 K to 373 K. Experimental results were correlated with the Peng-Robinson equation of state with the two-parameter van der Waals mixing rule. At the same time, the Henry's coefficient, partial molar enthalpy change and partial molar entropy change of CO2 during dissolution at different temperature were also calculated. 展开更多
关键词 carbon dioxide Methyl propionate Propyl propionate Vapor-liquid equilibrium data Henry's coefficient
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Extraction of Perilla Seed Oil Using Supercritical Carbon Dioxide and GC-MS Analysis 被引量:5
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作者 杨丽嫔 周游 +2 位作者 耿姗姗 刘末 雷红 《Agricultural Science & Technology》 CAS 2017年第8期1509-1512,共4页
[Objective] This study was aimed to determine the optimal parameters for the extraction of perilla seed oil to obtain high-quality perilla seed oil and analyze its compositions. [Method] In this study, perilla seed oi... [Objective] This study was aimed to determine the optimal parameters for the extraction of perilla seed oil to obtain high-quality perilla seed oil and analyze its compositions. [Method] In this study, perilla seed oil was extracted using supercritical CO2 (SC-CO2). The effects of extraction time, temperature and pressure were investigated by single-factor experiments and orthogonal array testing (ORT). The chemical compositions of extracted perilla seed oil were investigated by GC-MS. [Result] The optimal conditions for the extraction of perilla seed oil using SC-CO2 were extraction time of 4 h, extraction temperature at 40 ℃, and extraction pressure at 23 MPa. Under these conditions, the extraction yield of perilla seed oil was maximized to 12.43%. GC-MS analysis revealed that perilla seed oil was a complex mixture containing 76.183% α-linolenic acid. [Conclusion] Supercritical CO2 extraction was proven to be an effective technology to extract oil from perilla seed, and GCMS was also a satisfactory method for analyzing the compositions of perilla seed oil. 展开更多
关键词 Perilla seed essential oil Supercritical carbon dioxide extraction Or-thogonal array testing (OAT) GC-MS
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