Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting t...Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting two greenhouse gases(methane and carbon dioxide)into syngas and its promising industrial applications.Nickel(Ni)-based catalysts,with high catalytic activity,low cost,and abundant resources,are considered ideal candidates for industrial applications.In this article,three reaction kinetic models were briefly introduced,namely the Power-Law(PL)model,the Eley-Rideal(ER)model,and the Langmuir-Hinshelwood-Hougen-Watson(LHHW)model.Based on the LHHW model,the reaction kinetics and mechanisms of different catalytic systems were systematically discussed,including the properties of supports,the doping of noble metals and transition metals,the role of promoters,and the influence of the geometric and electronic structures of Ni on the reaction mechanism.Furthermore,the kinetics of carbon deposition and elimination on various catalysts were analyzed.Based on the reaction rate expressions for carbon elimination,the reasons for the high activity of transition metal iron(Fe)-doped catalysts and core-shell structured catalysts in carbon elimination were explained.Based on the detailed collation and comparative analysis of the reaction mechanisms and kinetic characteristics across diverse Ni-based catalytic systems,a theoretical guidance for the designing of high-performance catalysts was provided in this work.展开更多
Artificial synthesis is an environment friendly photocatalytic strategy to converse carbon dioxide(CO_(2))into useful chemicals.However,water(H_(2)O)splitting,producing(hydrogen)H_(2) strongly,is always a competitive ...Artificial synthesis is an environment friendly photocatalytic strategy to converse carbon dioxide(CO_(2))into useful chemicals.However,water(H_(2)O)splitting,producing(hydrogen)H_(2) strongly,is always a competitive reaction to CO_(2) conversion.Therefore,proper cocatalysts are generally needed to enhance CO_(2) conversion but suppress H_(2) production.In this work,zinc/gallium(Zn/Ga)dual co-catalysts consisting of Zn0 and amorphous ZnGa_(2)O_(4) species were found to selectively produce carbon monoxide(CO)during the photocatalytic conversion of carbon dioxide(CO_(2))using water(H_(2)O)as an electron donor over photocatalysts such as NaTaO_(3),Ga_(2)O_(3),and ZnGa_(2)O_(4),and in the electrochemical reduction of CO_(2) over Zn0 electrodes.It is considered that there are two effects associated with the Zn/Ga dual co-catalysts:(1)a galvanic cell effect between Zn0 and amorphous ZnGa_(2)O_(4),and(2)a Z-scheme effect in NaTaO_(3)/Zn0/amorphous ZnGa_(2)O_(4).The coupling of these two effects favored the active and selective evolution of CO during the photocatalytic conversion of CO_(2) by H_(2)O.In the case of Ga_(2)O_(3) photocatalyst,480.8μmol/h of CO was produced with the presence of Zn/Ga dual cocatalysts.Moreover,the Zn/Ga dual cocatalysts universally worked in the electrochemical reduction of CO_(2).The partial current toward CO_(2) conversion was increased from 2.6 to 6.6 mA/cm,and the selectivity toward CO was promoted to from 46.4%to 74.2%.展开更多
Photocatalytic carbon dioxide reduction reaction(CO_(2)RR)is a carbon-neutral strategy to address global energy use and its impact on climate.Metal oxide and metal chalcogenide catalysts are the most investigated cata...Photocatalytic carbon dioxide reduction reaction(CO_(2)RR)is a carbon-neutral strategy to address global energy use and its impact on climate.Metal oxide and metal chalcogenide catalysts are the most investigated catalysts for photocatalytic CO_(2)RR.Unfortunately,low CO_(2)adsorption ability and limited active sites of metal oxide and metal chalcogenide catalysts for CO_(2)RR make them less competitive compared to their industrial counterparts.Inspired by applications of porphyrin-based metal-organic framework(MOF)catalysts for hydrogen evolution and photodynamic therapy,the investigations of these porphyrin-based MOFs,including pristine and composite porphyrin-based MOFs in photocatalytic CO_(2)RR,have attracted significant attention in the last five years due to their excellent CO_(2)adsorption capacities,high porosity,high stability,exceptional optoelectronic properties,and multi-functionality.However,due to the difference in photocatalytic CO_(2)RR,several critical issues need to be addressed to achieve the rational design of advanced porphyrin-based MOF photocatalysts to improve activity,selectivity,and stability for CO_(2)RR.Here,we review recent developments in the field of porphyrin-based MOF CO_(2)RR photocatalysts,along with critical issues,challenges,and perspectives concerning porphyrin-based MOF catalysts for photocatalytic CO_(2)RR.展开更多
As the core of cathode materials,sensitive metals play important roles in the optimization of acetate production from carbon dioxide(CO_(2))in microbial electrochemical system(MES).In this work,iron(Fe),copper(Cu),and...As the core of cathode materials,sensitive metals play important roles in the optimization of acetate production from carbon dioxide(CO_(2))in microbial electrochemical system(MES).In this work,iron(Fe),copper(Cu),and nickel(Ni)as sensitive metal cathode materials were evaluated for CO_(2) conversion in MES.The MES with Feelectrode as a promising electrode material demonstrated a superior CO_(2) reduction performance with a maximum acetate accumulation of 417.9±39.2 mg/L,which was 1.5 and 1.7 folds higher than that in the Ni-electrode and Cu-electrode groups,respectively.Furthermore,an outstanding electron recovery efficiency of 67.7%was shown in the Fe-electrode group.The electron transfer between electrode-suspended sludge was systematically cross-evaluated by the electrochemical behavior and extracellular polymeric substances.The Fe-electrode group had the highest electron transfer rate with 0.194 s-1(k_(app)),which was 17.6 and 21.5 times higher than that of the Cu-and Ni-electrode groups,respectively.Fe-electrode was beneficial for reducing electrochemical impedance between the electrode and suspended sludge.Additionally,redox substances in extracellular polymeric substances of the Fe-electrode group were increased,implying more favorable electron transport dynamics.Simultaneously,enrichments of functional bacteria Acetoanerobium and increased key enzymes involved in the carbonyl pathway of the Fe-electrode group were observed,which also promoted CO_(2) conversion in MES.This study provides a perspective on evaluating the promising sensitive metal electrode material for the process of CO_(2) valorization in MES and offers a reference for the subsequent electrode modification.展开更多
The photocatalytic reduction of CO_(2)is a crucial area of research aimed at addressing the dual challenges of mitigating rising CO_(2)emissions and producing sustainable chemical feedstocks.While multielectron reduct...The photocatalytic reduction of CO_(2)is a crucial area of research aimed at addressing the dual challenges of mitigating rising CO_(2)emissions and producing sustainable chemical feedstocks.While multielectron reduction pathways for CO_(2)are well explored,the single electron reduction to produce the highly reactive carbon dioxide radical anion(CO_(2)^(·-))remains challenging yet promising for green organic transformations.This review contributes to the field by providing a comprehensive analysis of the mechanisms,materials,and reaction pathways involved in CO_(2)^(·-)generation,focusing on the use of visible-lightdriven photocatalytic materials to circumvent the need for high-energy ultraviolet irradiation.Through a systematic examination of CO_(2)^(·-)production,detection methods,and chemical utilization in photocatalytic carboxylation reactions,this review advances understanding of the chemistry of CO_(2)^(·-)and its applications in sustainable chemical synthesis.In addition,it highlights existing key challenges,such as redox potential limitations,and proposes strategies for scaling up photocatalytic systems to enable practical application.By illuminating the pathway to effectively photocatalyze CO_(2)^(·-)generation and its transformative potential in sustainable chemical synthesis,this review equips scientists with critical insights and strategic approaches for overcoming current limitations,driving innovation in photocatalytic materials for solar-to-chemical energy conversion.展开更多
Morphology and growth rate of carbon dioxide hydrate on the interface between liquid carbon dioxide and humic acid solutions were studied in this work.It was found that after the growth of the hydrate film at the inte...Morphology and growth rate of carbon dioxide hydrate on the interface between liquid carbon dioxide and humic acid solutions were studied in this work.It was found that after the growth of the hydrate film at the interface,further growth of hydrate due to the suction of water in the capillary system formed between the wall of the cuvette and the end boundary of the hydrate layer occurs.Most probably,substantial effects on the formation of this capillary system may be caused by variations in reactor wall properties,for example,hydrophobic-hydrophilic balance,roughness,etc.We found,that the rate of CO_(2) hydrate film growth on the surface of the humic acid aqueous solution is 4-fold to lower in comparison with the growth rate on the surface of pure water.We suppose that this is caused by the adsorption of humic acid associates on the surface of hydrate particles and,as a consequence,by the deceleration of the diffusion of dissolved carbon dioxide to the growing hydrate particle.展开更多
Nitrogen-doped activated carbon(N-AC)was successfully prepared by KOH-activation and nitrogen doping using ammonia(NH3)heat treatment.Coconut shell-derived activated carbon(AC)was heat-treated under NH3 gas in the tem...Nitrogen-doped activated carbon(N-AC)was successfully prepared by KOH-activation and nitrogen doping using ammonia(NH3)heat treatment.Coconut shell-derived activated carbon(AC)was heat-treated under NH3 gas in the temperature range of 700℃-900℃.Likewise,the mixture of potassium hydroxide(KOH)and AC was heated at 800℃,followed by heat treatment underNH3 gas at 800℃(hereafter referred to asKOH-N-AC800).Scanning electron microscopy(SEM),Raman spectroscopy,X-ray photoelectron spectroscopy(XPS)and Brunauer-Emmett-Teller(BET)method were utilized to analyze morphology,crystallinity,chemical bonding,chemical composition and surface area.The surface area and porosity of N-AC increased with increasing NH3 heat treatment.Similarly,the nitrogen content in the N-AC increased from 3.23%to 4.84 at%when the NH3 heat treatment was raised from 700℃ to 800℃.However,the nitrogen content of N-AC decreased to 3.40 at% after using NH3 heat treatment at 900℃.The nitrogen content of KOH-N-AC800 is 5.43 at%.KOH-N-AC800 and N-AC800 exhibited improvements of 33.66% and 26.24%,respectively,in CO_(2) adsorption compared with AC.The enhancement of CO_(2) adsorption of KOH-N-AC800 is attributed to the synergic effect of the nitrogen doping,high surface area,and porosity.The results exhibited that nitrogen sites on the surface play a more significant role in CO_(2) adsorption than surface area and porosity.This work proposes the potential synergistic effect of KOH-activation and nitrogen doping for enhancing the CO_(2) adsorption capacity of activated carbon.展开更多
A single component molybdenum catalyst was synthesized and its activity in the cycloaddition reaction of CO_(2)and epoxide was tested.The results show that the molybdenum catalysts exhibit high activity and a broad su...A single component molybdenum catalyst was synthesized and its activity in the cycloaddition reaction of CO_(2)and epoxide was tested.The results show that the molybdenum catalysts exhibit high activity and a broad substrate scope under the reaction conditions of 80℃and 0.5 MPa of CO_(2),solvent-free,and and no nucleophilic cocatalysts,affording a wide range of cyclic carbonates in yields of 42%~94%.The reaction mechanism was investigated using in situ infrared(in situ IR),high-resolution mass spectrometry(HRMS)and Fourier transform infrared spectroscopy(FT-IR).展开更多
This study reviews the recent progress and trends of carbon capture,utilization and storage(CCUS)technologies,with a particular focus on related policy orientations,technological status,and representative projects acr...This study reviews the recent progress and trends of carbon capture,utilization and storage(CCUS)technologies,with a particular focus on related policy orientations,technological status,and representative projects across North America,Europe,the Middle East,and China.The technical connotations of CCUS are elucidated,and the existing issues and challenges are identified from the perspectives of technology,economics,safety and system integration.The CO_(2) capture technologies are relatively mature;the emergence of novel processes such as direct air capture(DAC)and advanced materials such as metal-organic frameworks(MOFs)offer new choices for efficient capture,but issues related to high energy consumption and operational costs remain unresolved.The CO_(2) geological utilization has developed earlier,where breakthroughs rely on effective source matching,enhanced miscibility and increased swept volume.The CO_(2) chemical utilization exhibits broad market potential for producing high value-added products,and the development of catalytic systems with high conversion efficiency and low cost is identified as the core challenge.For CO_(2) storage,diverse geological bodies provide vast theoretical capacities on both land and offshore worldwide,but subsidy policies and carbon market regulation are required to offset the limited economic returns of storage technologies.This study highlights several frontier technologies,including low-concentration CO_(2) capture,CO_(2)-enhanced oil recovery(EOR),CO_(2)-based green fuel synthesis,microbial CO_(2) conversion,CO_(2) mineralization and hydrogen production,and CO_(2) cushion gas replacement in underground gas storage(UGS).Through cost-effective innovation,regional pipeline network development,flexible technology integration,coordinated macro-policy regulation,and cross-disciplinary collaboration,CCUS can achieve a transformative scale-up from million-ton and ten-million-ton capacities to the hundred-million-ton level,contributing to the achievement of the carbon neutrality goals of China.展开更多
A strategy for copper-catalyzed and biphosphine ligand controlled boracarboxylation of 1,3-dienes and CO_(2) with 3,4-selectivity was developed.The Cu Cl coupled with DPPF(1,1-bis(diphenylphosphino)ferrocene)was assig...A strategy for copper-catalyzed and biphosphine ligand controlled boracarboxylation of 1,3-dienes and CO_(2) with 3,4-selectivity was developed.The Cu Cl coupled with DPPF(1,1-bis(diphenylphosphino)ferrocene)was assigned to be the best catalyst,with 84%yield and exclusive3,4-selectivity.The ligand effect on both catalytic activity and regioselectivity of boracarboxylation was disclosed,which is rarely reported in any copper catalyzed boracarboxylation.The borocupration process is revealed to be a vital step for the biphosphine participated boracarboxylation of 1,3-dienes with CO_(2).The minimal substrate distortion occurring in 3,4-borocupration favors the 3,4-regioselectivity of boracarboxylation.The“pocket”confinement and suitableβ_(n)(92°–106°)of bisphosphine ligands are demonstrated to be in favour of the interaction between LCu-Bpin complex(the catalytic precursor)and1,3-diene substrate to decrease their interaction energyΔE_(int)(ζ)in 3,4-borocupration,thus promoting the 3,4-boracarboxylation.展开更多
Using thermogravimetric experiments,the kinetic characteristics of magnesite thermal decomposition were investigated under the condition of 10%(vol) CO_(2) in the actual production atmosphere of an entrained-flow dyna...Using thermogravimetric experiments,the kinetic characteristics of magnesite thermal decomposition were investigated under the condition of 10%(vol) CO_(2) in the actual production atmosphere of an entrained-flow dynamic roasting furnace.Based on a multi-method collaborative framework,the three kinetic factors in the magnesite thermal decomposition process were systematically calculated through parameter cross-verification between the Hu-Gao-Zhang integral method and the Kissinger differential method.The kinetic mechanism was initially screened by the double equal and double step method and further determined by combining with the Malek maximum probability method.The study revealed that CO_(2) in the atmosphere exerts an inhibitory effect on the decomposition of carbonate species within magnesite.Furthermore,the presence of impurities(e.g.,calcium carbonate)was found to interfere with the determination of reaction mechanisms via Malek's method at elevated temperatures.The results show that in a 10%(vol)CO_(2)atmosphere,the main decomposition temperature of magnesite ranges from 550℃ to 650℃,the average activation energy is 66.00 k J·mol^(-1),the pre-exponential factor is 1.05×10^(5)s^(-1),and the decomposition process conforms to the random nucleation and growth model.展开更多
Power consumption increases annually,wherefore the air emissions during its production occasionally increase.One of the most promising trends of environmentally safe generation of electricity is the transition to oxyg...Power consumption increases annually,wherefore the air emissions during its production occasionally increase.One of the most promising trends of environmentally safe generation of electricity is the transition to oxygen-fuel power complexes operating on a carbon dioxide working medium,with a share of its capture up to 99%.It is worth noting that the breadth of application of power technologies is determined not only on the basis of criteria of thermal efficiency and environmental safety.The most important criterion is the indicator of economic accessibility,the failure of which does not yet allow for a large-scale transition to the use of electric power technologies with the capture and disposal of greenhouse gases.In this study,a set of multifactorial models for estimating the cost of the main generating equipment operating on supercritical carbon dioxide has been developed.it is found that an increase in the initial temperature and pressure will increase the cost of the main generating equipment operating on supercritical carbon dioxide.展开更多
Laparoscopic liver resection(LLR)is currently the first-linetreatment for multiple liver diseases.Although clinical data have proven its safety and effectiveness,bleeding and carbon dioxide(CO_(2))embolism are still t...Laparoscopic liver resection(LLR)is currently the first-linetreatment for multiple liver diseases.Although clinical data have proven its safety and effectiveness,bleeding and carbon dioxide(CO_(2))embolism are still the major complications of LLR.The objective of this review was to summarize the pathogenetic mechanism,clinical manifestations,risk factors,prophylactic measures,and treatment strategies for CO_(2) embolism in LLR and propose further research directions regarding these controversial issues.A narrative review of the literature from three databases,including PubMed,Embase,and Web of Science,was conducted without any date or language restrictions.The search terms included CO_(2) embolism,gas embolism,laparoscopy,liver resection,and hepatectomy.The incidence of CO_(2) embolism in LLR(1.2%–4.6%)is approximately 10 times greater than that in overall laparoscopic surgery(0.15%).Transesophageal echocardiogram is currently considered the gold standard for identifying CO_(2) embolism.Risk factors are multifactorial and involve patient characteristics,procedural techniques,and anesthetic management.Presently,in clinical practice,a pneumoperitoneal pressure of 10–15 mmHg is typically used to balance bleeding and CO_(2) embolism during LLR.The majority of observed CO_(2) embolism events are benign,with no significantclinical impact on short-term or long-term outcomes.However,meticulous monitoring,timely recognition,and prompt intervention are crucial during LLR to prevent life-threatening events.Future research should further refinerisk stratification,validate early detection methods,and develop standardized management protocols for CO_(2) embolism in LLR.展开更多
Sepsis management has significantly improved over the past decades,with intensivists playing a pivotal role in its identification and treatment.[1,2]However,resource constraints in large tertiary hospitals in China li...Sepsis management has significantly improved over the past decades,with intensivists playing a pivotal role in its identification and treatment.[1,2]However,resource constraints in large tertiary hospitals in China limit patient admissions,leading to overcrowding in the emergency departments(EDs)with critically ill patients.[3]This highlights the urgent need for enhanced risk stratification and optimized sepsis management in emergency settings.展开更多
Carbon dioxide photocatalytic reduction (CO_(2)-PR) is an efficient method for controlling CO_(2)emissions and generating cleaner energy while mitigating global warming.Tungsten oxides (WxOy) have attracted considerab...Carbon dioxide photocatalytic reduction (CO_(2)-PR) is an efficient method for controlling CO_(2)emissions and generating cleaner energy while mitigating global warming.Tungsten oxides (WxOy) have attracted considerable attention for CO_(2)-PR due to their excellent spectral absorbance.However,comprehensive reviews are lacking on the use of WxOyfor CO_(2)-PR.Therefore,this review provides a detailed summary of t research progress made with WxOy-based catalysts in CO_(2)-PR.It also explains the fundamental principles of CO_(2)-PR and evaluates key performance indicators that affect the activity of WxOy-based photocatalysts,including yield,selectivity,stability,and apparent quantum yield.Additionally,this review explores opportunities for synthesizing high-performance WxOy-based photocatalysts and highlights their potential for the green preparation of C1/C2 products through CO_(2)-PR.These innovative strategies aim to address the challenges and pressures associated with energy and environmental issues,particularly by enhancing artificial photosynthesis efficiency.展开更多
Mechanical alterations in shale formations due to exposure to water-based fracturing fluids and supercritical carbon dioxide(ScCO_(2))significantly affect the performance of shale gas exploration and CO_(2) geo-seques...Mechanical alterations in shale formations due to exposure to water-based fracturing fluids and supercritical carbon dioxide(ScCO_(2))significantly affect the performance of shale gas exploration and CO_(2) geo-sequestration.In this study,a hydrothermal(HT)reaction system was set up to treat Longmaxi shale samples of varying mineralogies(carbonate-,clay-,and quartz-rich)with different fluids,i.e.deionized(DI)water,2%potassium chloride(KCl)solution,and ScCO_(2) under HT conditions expected in shale formation.Statistical micro-indentation was conducted to characterize the mechanical property alterations caused by the shale-fluid interactions.An in situ morphological and mineralogical identification technique that combines scanning electron microscopy(SEM)and backscattered electron(BSE)imaging with energy-dispersive X-ray spectroscopy(EDS)was used to analyze the microstructural and mineralogical changes of the treated shale samples.Results show no apparent changes in the Young's modulus,E,and hardness,H,after treatment with DI water under room temperature(20℃)and atmospheric pressure for 7 d.In contrast,E and H were decreased by 31.2%and 37.5%at elevated temperature(80℃)and pressure(8 MPa),respectively.The addition of 2%KCl into DI water mitigated degradation of the mechanical properties.Quartz-rich shale specimens are the least sensitive to the water-based fracturing fluids,followed by the clay-rich and carbonate-rich shale formations.Based on in situ morphological and mineralogical identification,the primary factors for the mechanical degradation induced by water-based fluids include carbonate dissolution,clay swelling,and pyrite oxidation.Slight increases in the measured E and H and compression of porous clay aggregates were observed after treatment with ScCO_(2).The major factor contributing to the mechanical changes resulting from the exposure to scCO_(2) appears to be the competition between swelling caused by adsorption and compression of shale matrix.展开更多
Dimensionality has great influence on the photo/electro-catalysts properties of covalent organic frameworks(COFs) because of the different electronic and porous structures.However,very rare attention has been paid on ...Dimensionality has great influence on the photo/electro-catalysts properties of covalent organic frameworks(COFs) because of the different electronic and porous structures.However,very rare attention has been paid on the dimensionality and function correlations of COF materials.In the present work,one new two-dimensional phthalocyanine COF,namely 2D-NiPc-COF,and one new three-dimensional phthalocyanine COF,namely 3D-NiPc-COF,were fabricated according to the imide reaction between tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(Ⅱ) with [2,2-bipyridine]-5,5-diamine and tetrakis(4-aminophenyl) methane,respectively.The crystalline structures of both COFs are verified by the powder X-ray diffraction analysis,computational simulation,and high resolution transmission electron microscopy measurement.Notably,3D-NiPc-COF with dispersed conjugated modules has high utilization efficiency of NiPc electroactive sites of 26.8%,almost two times higher than the in-plane stacking2D-NiPc-COF measured by electrochemical measurement,in turn resulting in its superior electrocatalytic performance with high CO_(2)-to-CO Faradaic efficiency over 90% in a wide potential window,a large partial CO current density of-13.97 mA/cm^(2) at-0.9 V(vs.reversible hydrogen electrode) to 2D-NiPc-COF.Moreover,3D-NiPc-COF has higher turnover number and turnover frequency of 5741.6 and 0.18 s^(-1) at-0.8 V during 8 h lasting measurement.The present work provides an example for the investigation on the correlation between dimensionality and electrochemical properties of 2D and 3D phthalocyanine COFs.展开更多
The increasing level of atmospheric carbon dioxide(CO_(2))caused by intensified human activities has exacerbated the greenhouse effect,calling for the technology of CO_(2)fixation.Among the proposed technologies,elect...The increasing level of atmospheric carbon dioxide(CO_(2))caused by intensified human activities has exacerbated the greenhouse effect,calling for the technology of CO_(2)fixation.Among the proposed technologies,electrocatalytic CO_(2)reduction in acidic electrolytes has garnered significant attention for its potential in sustainable carbon utilization and renewable energy storage.This review provides a summary of recent advancements in acidic CO_(2)reduction,with a focus on catalyst design strategies,the optimization of the local reaction environment,and the effect of cations.We first evaluated the performance and discussed the challenges for acidic CO_(2)reduction in H-type cells,flow cells,and membrane electrode assembly.Afterward,we highlight the innovative strategies for promoting CO_(2)reduction through optimizing the intrinsic activity and regulating the local environment of catalysts.The critical role of cations in enhancing CO_(2)reduction selectivity is also discussed.The review concludes with an outlook on future research directions,especially the need for the design of catalysts and systems that are stable,scalable,and highly efficient.展开更多
The calcium-containing rare earth solution is generated during the recovery processes of NdFeB waste,which is treated as wastewater by enterprises.In this paper,the carbon dioxide carbonization method was applied to t...The calcium-containing rare earth solution is generated during the recovery processes of NdFeB waste,which is treated as wastewater by enterprises.In this paper,the carbon dioxide carbonization method was applied to the separation of rare earths and calcium in the solution,as well as the preparation of rare earth oxides with a large specific surface.It is shown that the process of CO_(2)carbonization of solution includes reactions such as the dissolution,diffusion and ionization of CO_(2),the carbonate precipitation of rare earth ions,and the neutralization of hydrogen ions.At a pH of 4.5,the carbonization precipitation rate is effectively controlled,enabling homogeneous precipitation and ensuring both high precipitation yield and rare earth oxides purity.In this way,the crystallization of carbonization products is a process dominated by the oriented attachment theory and coexisting with the Ostwald ripening theory,resulting in abundant pores formed by multiple layers of stacking in the products.With the optimal carbonization conditions,the rare earth precipitation yield solution reaches 99.32%.The obtained carbonization products are crystalline(LaCe)(CO_(3))_(3)·8H_(2)O,and the purity of the rare earth oxides is as high as 99.22 wt%.The specific surface area of the rare earth oxides reaches 94.7 m^(2)/g,and its adsorption efficiency for tetracycline hydrochloride in solution can reach 92.6%in a short time.The rare earth oxides are expected to be used as an adsorption material for wastewater treatment and other adsorption environments.展开更多
This study investigates the application of carbon dioxide (CO2) sequestration to address challenges in water-drive gas reservoirs, specifically focusing on improving gas recovery and mitigating water invasion. Traditi...This study investigates the application of carbon dioxide (CO2) sequestration to address challenges in water-drive gas reservoirs, specifically focusing on improving gas recovery and mitigating water invasion. Traditional methods like blow-down and co-production have limitations, including sand production, water coning, and inefficiency in strong aquifers. To overcome these issues, this research explores CO2 injection near the edge aquifer, aiming to reduce water influx and enhance gas recovery through the propagation of a CO2 plume in the gas-water contact zone. Both synthetic and real compositional reservoir models were studied, with CO2 injection performed while maintaining reservoir pressure below 90% of the initial level. Results show that CO2 sequestration significantly improved recovery, particularly in higher permeability reservoirs, where it reduced aquifer influx and increased gas production by 26% under challenging conditions. While CO2 dissolution in water decreased aquifer influx by 39%, its adverse effect on sweep efficiency led to a reduction in gas and water production by 4.2% and 10%, respectively. The method's effectiveness was not significantly impacted by aquifer permeability, but it was sensitive to vertical-to-horizontal permeability ratios. When applied to a real gas reservoir, the proposed method increased gas production by 14% compared to conventional techniques, with minimal CO2 production over a 112-year period. This study demonstrates the potential of CO2 sequestration as a comprehensive solution for enhancing gas recovery, reducing water production, and mitigating environmental impacts in water-drive gas reservoirs.展开更多
基金Supported by Innovation Capability Support Program of Shaanxi(2024RS-CXTD-53,2024ZC-KJXX-096)the Key R&D Program of Shaanxi Province(2022QCY-LL-69)Xi’an Science and Technology Project(24GXFW0089)。
文摘Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting two greenhouse gases(methane and carbon dioxide)into syngas and its promising industrial applications.Nickel(Ni)-based catalysts,with high catalytic activity,low cost,and abundant resources,are considered ideal candidates for industrial applications.In this article,three reaction kinetic models were briefly introduced,namely the Power-Law(PL)model,the Eley-Rideal(ER)model,and the Langmuir-Hinshelwood-Hougen-Watson(LHHW)model.Based on the LHHW model,the reaction kinetics and mechanisms of different catalytic systems were systematically discussed,including the properties of supports,the doping of noble metals and transition metals,the role of promoters,and the influence of the geometric and electronic structures of Ni on the reaction mechanism.Furthermore,the kinetics of carbon deposition and elimination on various catalysts were analyzed.Based on the reaction rate expressions for carbon elimination,the reasons for the high activity of transition metal iron(Fe)-doped catalysts and core-shell structured catalysts in carbon elimination were explained.Based on the detailed collation and comparative analysis of the reaction mechanisms and kinetic characteristics across diverse Ni-based catalytic systems,a theoretical guidance for the designing of high-performance catalysts was provided in this work.
基金supported by the National Key R&D Program of China(No.2023YFC3710800)the National Natural Science Foundation of China(No.22376207)+1 种基金the Research Fund of High-Level Training Talents of“333”Project in Jiangsu provinceFunding for school-level research projects of Yancheng Institute of Technology(Nos.xjr2024008 and xjr2023055).
文摘Artificial synthesis is an environment friendly photocatalytic strategy to converse carbon dioxide(CO_(2))into useful chemicals.However,water(H_(2)O)splitting,producing(hydrogen)H_(2) strongly,is always a competitive reaction to CO_(2) conversion.Therefore,proper cocatalysts are generally needed to enhance CO_(2) conversion but suppress H_(2) production.In this work,zinc/gallium(Zn/Ga)dual co-catalysts consisting of Zn0 and amorphous ZnGa_(2)O_(4) species were found to selectively produce carbon monoxide(CO)during the photocatalytic conversion of carbon dioxide(CO_(2))using water(H_(2)O)as an electron donor over photocatalysts such as NaTaO_(3),Ga_(2)O_(3),and ZnGa_(2)O_(4),and in the electrochemical reduction of CO_(2) over Zn0 electrodes.It is considered that there are two effects associated with the Zn/Ga dual co-catalysts:(1)a galvanic cell effect between Zn0 and amorphous ZnGa_(2)O_(4),and(2)a Z-scheme effect in NaTaO_(3)/Zn0/amorphous ZnGa_(2)O_(4).The coupling of these two effects favored the active and selective evolution of CO during the photocatalytic conversion of CO_(2) by H_(2)O.In the case of Ga_(2)O_(3) photocatalyst,480.8μmol/h of CO was produced with the presence of Zn/Ga dual cocatalysts.Moreover,the Zn/Ga dual cocatalysts universally worked in the electrochemical reduction of CO_(2).The partial current toward CO_(2) conversion was increased from 2.6 to 6.6 mA/cm,and the selectivity toward CO was promoted to from 46.4%to 74.2%.
基金financially supported by the National Natural Science Foundation of China(No.22305009)the Science and Technology Development Fund,Macao SAR(File no.FDCT-0125/2022/A and FDCT-0006/2023/RIB1)Hong Kong Research Grant Council(RGC)General Research Fund(GRF)City U 11305419,11306920,CityU 11308721,CityU 11316522,and SIRG7020022。
文摘Photocatalytic carbon dioxide reduction reaction(CO_(2)RR)is a carbon-neutral strategy to address global energy use and its impact on climate.Metal oxide and metal chalcogenide catalysts are the most investigated catalysts for photocatalytic CO_(2)RR.Unfortunately,low CO_(2)adsorption ability and limited active sites of metal oxide and metal chalcogenide catalysts for CO_(2)RR make them less competitive compared to their industrial counterparts.Inspired by applications of porphyrin-based metal-organic framework(MOF)catalysts for hydrogen evolution and photodynamic therapy,the investigations of these porphyrin-based MOFs,including pristine and composite porphyrin-based MOFs in photocatalytic CO_(2)RR,have attracted significant attention in the last five years due to their excellent CO_(2)adsorption capacities,high porosity,high stability,exceptional optoelectronic properties,and multi-functionality.However,due to the difference in photocatalytic CO_(2)RR,several critical issues need to be addressed to achieve the rational design of advanced porphyrin-based MOF photocatalysts to improve activity,selectivity,and stability for CO_(2)RR.Here,we review recent developments in the field of porphyrin-based MOF CO_(2)RR photocatalysts,along with critical issues,challenges,and perspectives concerning porphyrin-based MOF catalysts for photocatalytic CO_(2)RR.
基金supported by the Science and Technology Commission of Shanghai Municipality Foundation(No.22230710500)the Interdisciplinary joint research project of Tongji University(No.2023-3-YB-07).
文摘As the core of cathode materials,sensitive metals play important roles in the optimization of acetate production from carbon dioxide(CO_(2))in microbial electrochemical system(MES).In this work,iron(Fe),copper(Cu),and nickel(Ni)as sensitive metal cathode materials were evaluated for CO_(2) conversion in MES.The MES with Feelectrode as a promising electrode material demonstrated a superior CO_(2) reduction performance with a maximum acetate accumulation of 417.9±39.2 mg/L,which was 1.5 and 1.7 folds higher than that in the Ni-electrode and Cu-electrode groups,respectively.Furthermore,an outstanding electron recovery efficiency of 67.7%was shown in the Fe-electrode group.The electron transfer between electrode-suspended sludge was systematically cross-evaluated by the electrochemical behavior and extracellular polymeric substances.The Fe-electrode group had the highest electron transfer rate with 0.194 s-1(k_(app)),which was 17.6 and 21.5 times higher than that of the Cu-and Ni-electrode groups,respectively.Fe-electrode was beneficial for reducing electrochemical impedance between the electrode and suspended sludge.Additionally,redox substances in extracellular polymeric substances of the Fe-electrode group were increased,implying more favorable electron transport dynamics.Simultaneously,enrichments of functional bacteria Acetoanerobium and increased key enzymes involved in the carbonyl pathway of the Fe-electrode group were observed,which also promoted CO_(2) conversion in MES.This study provides a perspective on evaluating the promising sensitive metal electrode material for the process of CO_(2) valorization in MES and offers a reference for the subsequent electrode modification.
基金funding programs,the Walter Benjamin Programme(DFG,German Research Foundation,project number:530742479)the ProChancecareer Programme for the Promotion of Equal Opportunities in Academia for providing the financial support+1 种基金financial support by the Deutsche Forschungsgemeinschaft via the TRR 234 Cata Light(DFG,German Research Foundation)-Projektnummer 364549901-TRR 234[B6]the financial support taken from the CSIR and UGC,Delhi,India。
文摘The photocatalytic reduction of CO_(2)is a crucial area of research aimed at addressing the dual challenges of mitigating rising CO_(2)emissions and producing sustainable chemical feedstocks.While multielectron reduction pathways for CO_(2)are well explored,the single electron reduction to produce the highly reactive carbon dioxide radical anion(CO_(2)^(·-))remains challenging yet promising for green organic transformations.This review contributes to the field by providing a comprehensive analysis of the mechanisms,materials,and reaction pathways involved in CO_(2)^(·-)generation,focusing on the use of visible-lightdriven photocatalytic materials to circumvent the need for high-energy ultraviolet irradiation.Through a systematic examination of CO_(2)^(·-)production,detection methods,and chemical utilization in photocatalytic carboxylation reactions,this review advances understanding of the chemistry of CO_(2)^(·-)and its applications in sustainable chemical synthesis.In addition,it highlights existing key challenges,such as redox potential limitations,and proposes strategies for scaling up photocatalytic systems to enable practical application.By illuminating the pathway to effectively photocatalyze CO_(2)^(·-)generation and its transformative potential in sustainable chemical synthesis,this review equips scientists with critical insights and strategic approaches for overcoming current limitations,driving innovation in photocatalytic materials for solar-to-chemical energy conversion.
基金supported by the Russian Science Foundation(23-29-00830).
文摘Morphology and growth rate of carbon dioxide hydrate on the interface between liquid carbon dioxide and humic acid solutions were studied in this work.It was found that after the growth of the hydrate film at the interface,further growth of hydrate due to the suction of water in the capillary system formed between the wall of the cuvette and the end boundary of the hydrate layer occurs.Most probably,substantial effects on the formation of this capillary system may be caused by variations in reactor wall properties,for example,hydrophobic-hydrophilic balance,roughness,etc.We found,that the rate of CO_(2) hydrate film growth on the surface of the humic acid aqueous solution is 4-fold to lower in comparison with the growth rate on the surface of pure water.We suppose that this is caused by the adsorption of humic acid associates on the surface of hydrate particles and,as a consequence,by the deceleration of the diffusion of dissolved carbon dioxide to the growing hydrate particle.
基金funded by Burapha University,grant number SDG 4/2568.
文摘Nitrogen-doped activated carbon(N-AC)was successfully prepared by KOH-activation and nitrogen doping using ammonia(NH3)heat treatment.Coconut shell-derived activated carbon(AC)was heat-treated under NH3 gas in the temperature range of 700℃-900℃.Likewise,the mixture of potassium hydroxide(KOH)and AC was heated at 800℃,followed by heat treatment underNH3 gas at 800℃(hereafter referred to asKOH-N-AC800).Scanning electron microscopy(SEM),Raman spectroscopy,X-ray photoelectron spectroscopy(XPS)and Brunauer-Emmett-Teller(BET)method were utilized to analyze morphology,crystallinity,chemical bonding,chemical composition and surface area.The surface area and porosity of N-AC increased with increasing NH3 heat treatment.Similarly,the nitrogen content in the N-AC increased from 3.23%to 4.84 at%when the NH3 heat treatment was raised from 700℃ to 800℃.However,the nitrogen content of N-AC decreased to 3.40 at% after using NH3 heat treatment at 900℃.The nitrogen content of KOH-N-AC800 is 5.43 at%.KOH-N-AC800 and N-AC800 exhibited improvements of 33.66% and 26.24%,respectively,in CO_(2) adsorption compared with AC.The enhancement of CO_(2) adsorption of KOH-N-AC800 is attributed to the synergic effect of the nitrogen doping,high surface area,and porosity.The results exhibited that nitrogen sites on the surface play a more significant role in CO_(2) adsorption than surface area and porosity.This work proposes the potential synergistic effect of KOH-activation and nitrogen doping for enhancing the CO_(2) adsorption capacity of activated carbon.
文摘A single component molybdenum catalyst was synthesized and its activity in the cycloaddition reaction of CO_(2)and epoxide was tested.The results show that the molybdenum catalysts exhibit high activity and a broad substrate scope under the reaction conditions of 80℃and 0.5 MPa of CO_(2),solvent-free,and and no nucleophilic cocatalysts,affording a wide range of cyclic carbonates in yields of 42%~94%.The reaction mechanism was investigated using in situ infrared(in situ IR),high-resolution mass spectrometry(HRMS)and Fourier transform infrared spectroscopy(FT-IR).
基金Supported by the Major Project of the National Social Science Fund of China(24&ZD106)National Science and Technology Major Project on New Oil and Gas Exploration and Development(205ZD1406807)Soft Science Research Project of CNPC(20250110-4).
文摘This study reviews the recent progress and trends of carbon capture,utilization and storage(CCUS)technologies,with a particular focus on related policy orientations,technological status,and representative projects across North America,Europe,the Middle East,and China.The technical connotations of CCUS are elucidated,and the existing issues and challenges are identified from the perspectives of technology,economics,safety and system integration.The CO_(2) capture technologies are relatively mature;the emergence of novel processes such as direct air capture(DAC)and advanced materials such as metal-organic frameworks(MOFs)offer new choices for efficient capture,but issues related to high energy consumption and operational costs remain unresolved.The CO_(2) geological utilization has developed earlier,where breakthroughs rely on effective source matching,enhanced miscibility and increased swept volume.The CO_(2) chemical utilization exhibits broad market potential for producing high value-added products,and the development of catalytic systems with high conversion efficiency and low cost is identified as the core challenge.For CO_(2) storage,diverse geological bodies provide vast theoretical capacities on both land and offshore worldwide,but subsidy policies and carbon market regulation are required to offset the limited economic returns of storage technologies.This study highlights several frontier technologies,including low-concentration CO_(2) capture,CO_(2)-enhanced oil recovery(EOR),CO_(2)-based green fuel synthesis,microbial CO_(2) conversion,CO_(2) mineralization and hydrogen production,and CO_(2) cushion gas replacement in underground gas storage(UGS).Through cost-effective innovation,regional pipeline network development,flexible technology integration,coordinated macro-policy regulation,and cross-disciplinary collaboration,CCUS can achieve a transformative scale-up from million-ton and ten-million-ton capacities to the hundred-million-ton level,contributing to the achievement of the carbon neutrality goals of China.
基金the National Key R&D Program of China(No.2022YFB4101900)National Natural Science Foundation of China(Nos.22278305,U21B2096)Natural Science Foundation of Tianjin City(No.23JCZDJC00040)。
文摘A strategy for copper-catalyzed and biphosphine ligand controlled boracarboxylation of 1,3-dienes and CO_(2) with 3,4-selectivity was developed.The Cu Cl coupled with DPPF(1,1-bis(diphenylphosphino)ferrocene)was assigned to be the best catalyst,with 84%yield and exclusive3,4-selectivity.The ligand effect on both catalytic activity and regioselectivity of boracarboxylation was disclosed,which is rarely reported in any copper catalyzed boracarboxylation.The borocupration process is revealed to be a vital step for the biphosphine participated boracarboxylation of 1,3-dienes with CO_(2).The minimal substrate distortion occurring in 3,4-borocupration favors the 3,4-regioselectivity of boracarboxylation.The“pocket”confinement and suitableβ_(n)(92°–106°)of bisphosphine ligands are demonstrated to be in favour of the interaction between LCu-Bpin complex(the catalytic precursor)and1,3-diene substrate to decrease their interaction energyΔE_(int)(ζ)in 3,4-borocupration,thus promoting the 3,4-boracarboxylation.
基金supported by the Natural Science Foundation of Liaoning Province(2024-MSLH-360)。
文摘Using thermogravimetric experiments,the kinetic characteristics of magnesite thermal decomposition were investigated under the condition of 10%(vol) CO_(2) in the actual production atmosphere of an entrained-flow dynamic roasting furnace.Based on a multi-method collaborative framework,the three kinetic factors in the magnesite thermal decomposition process were systematically calculated through parameter cross-verification between the Hu-Gao-Zhang integral method and the Kissinger differential method.The kinetic mechanism was initially screened by the double equal and double step method and further determined by combining with the Malek maximum probability method.The study revealed that CO_(2) in the atmosphere exerts an inhibitory effect on the decomposition of carbonate species within magnesite.Furthermore,the presence of impurities(e.g.,calcium carbonate)was found to interfere with the determination of reaction mechanisms via Malek's method at elevated temperatures.The results show that in a 10%(vol)CO_(2)atmosphere,the main decomposition temperature of magnesite ranges from 550℃ to 650℃,the average activation energy is 66.00 k J·mol^(-1),the pre-exponential factor is 1.05×10^(5)s^(-1),and the decomposition process conforms to the random nucleation and growth model.
基金This study conducted by Moscow Power Engineering Institute was financially supported by the Ministry of Science and Higher Education of the Russian Federation(project No.FSWF-2023-0014,contract No.075-03-2023-383,2023/18/01).
文摘Power consumption increases annually,wherefore the air emissions during its production occasionally increase.One of the most promising trends of environmentally safe generation of electricity is the transition to oxygen-fuel power complexes operating on a carbon dioxide working medium,with a share of its capture up to 99%.It is worth noting that the breadth of application of power technologies is determined not only on the basis of criteria of thermal efficiency and environmental safety.The most important criterion is the indicator of economic accessibility,the failure of which does not yet allow for a large-scale transition to the use of electric power technologies with the capture and disposal of greenhouse gases.In this study,a set of multifactorial models for estimating the cost of the main generating equipment operating on supercritical carbon dioxide has been developed.it is found that an increase in the initial temperature and pressure will increase the cost of the main generating equipment operating on supercritical carbon dioxide.
基金supported by grants from the Science and Technology Program of Zhejiang Province(Nos.2024C03201,2025C02133)the Central Government Guides Local Science and Technology Development Fund Projects(No.2024ZY01020).
文摘Laparoscopic liver resection(LLR)is currently the first-linetreatment for multiple liver diseases.Although clinical data have proven its safety and effectiveness,bleeding and carbon dioxide(CO_(2))embolism are still the major complications of LLR.The objective of this review was to summarize the pathogenetic mechanism,clinical manifestations,risk factors,prophylactic measures,and treatment strategies for CO_(2) embolism in LLR and propose further research directions regarding these controversial issues.A narrative review of the literature from three databases,including PubMed,Embase,and Web of Science,was conducted without any date or language restrictions.The search terms included CO_(2) embolism,gas embolism,laparoscopy,liver resection,and hepatectomy.The incidence of CO_(2) embolism in LLR(1.2%–4.6%)is approximately 10 times greater than that in overall laparoscopic surgery(0.15%).Transesophageal echocardiogram is currently considered the gold standard for identifying CO_(2) embolism.Risk factors are multifactorial and involve patient characteristics,procedural techniques,and anesthetic management.Presently,in clinical practice,a pneumoperitoneal pressure of 10–15 mmHg is typically used to balance bleeding and CO_(2) embolism during LLR.The majority of observed CO_(2) embolism events are benign,with no significantclinical impact on short-term or long-term outcomes.However,meticulous monitoring,timely recognition,and prompt intervention are crucial during LLR to prevent life-threatening events.Future research should further refinerisk stratification,validate early detection methods,and develop standardized management protocols for CO_(2) embolism in LLR.
基金supported by grants from the Chinese Academy of Medical Sciences Innovation Fund for Medical Sciences(2021-I2M-1-062,to BD).
文摘Sepsis management has significantly improved over the past decades,with intensivists playing a pivotal role in its identification and treatment.[1,2]However,resource constraints in large tertiary hospitals in China limit patient admissions,leading to overcrowding in the emergency departments(EDs)with critically ill patients.[3]This highlights the urgent need for enhanced risk stratification and optimized sepsis management in emergency settings.
基金supported by the National Natural Science Foundation of China(No.22376065)the Science and Technology Commission of Shanghai Municipality(No.22ZR1418600)Shanghai Municipal Science and Technology(No.20DZ2250400)。
文摘Carbon dioxide photocatalytic reduction (CO_(2)-PR) is an efficient method for controlling CO_(2)emissions and generating cleaner energy while mitigating global warming.Tungsten oxides (WxOy) have attracted considerable attention for CO_(2)-PR due to their excellent spectral absorbance.However,comprehensive reviews are lacking on the use of WxOyfor CO_(2)-PR.Therefore,this review provides a detailed summary of t research progress made with WxOy-based catalysts in CO_(2)-PR.It also explains the fundamental principles of CO_(2)-PR and evaluates key performance indicators that affect the activity of WxOy-based photocatalysts,including yield,selectivity,stability,and apparent quantum yield.Additionally,this review explores opportunities for synthesizing high-performance WxOy-based photocatalysts and highlights their potential for the green preparation of C1/C2 products through CO_(2)-PR.These innovative strategies aim to address the challenges and pressures associated with energy and environmental issues,particularly by enhancing artificial photosynthesis efficiency.
基金funded by the Open Research Fund Programof State Key Laboratory of Hydroscience and Engineering(Project Number:sklhse-2023-D-04)the National Natural Science Foundation of China(Grant Nos.51979144,51661165015,and 51323014).
文摘Mechanical alterations in shale formations due to exposure to water-based fracturing fluids and supercritical carbon dioxide(ScCO_(2))significantly affect the performance of shale gas exploration and CO_(2) geo-sequestration.In this study,a hydrothermal(HT)reaction system was set up to treat Longmaxi shale samples of varying mineralogies(carbonate-,clay-,and quartz-rich)with different fluids,i.e.deionized(DI)water,2%potassium chloride(KCl)solution,and ScCO_(2) under HT conditions expected in shale formation.Statistical micro-indentation was conducted to characterize the mechanical property alterations caused by the shale-fluid interactions.An in situ morphological and mineralogical identification technique that combines scanning electron microscopy(SEM)and backscattered electron(BSE)imaging with energy-dispersive X-ray spectroscopy(EDS)was used to analyze the microstructural and mineralogical changes of the treated shale samples.Results show no apparent changes in the Young's modulus,E,and hardness,H,after treatment with DI water under room temperature(20℃)and atmospheric pressure for 7 d.In contrast,E and H were decreased by 31.2%and 37.5%at elevated temperature(80℃)and pressure(8 MPa),respectively.The addition of 2%KCl into DI water mitigated degradation of the mechanical properties.Quartz-rich shale specimens are the least sensitive to the water-based fracturing fluids,followed by the clay-rich and carbonate-rich shale formations.Based on in situ morphological and mineralogical identification,the primary factors for the mechanical degradation induced by water-based fluids include carbonate dissolution,clay swelling,and pyrite oxidation.Slight increases in the measured E and H and compression of porous clay aggregates were observed after treatment with ScCO_(2).The major factor contributing to the mechanical changes resulting from the exposure to scCO_(2) appears to be the competition between swelling caused by adsorption and compression of shale matrix.
基金Financial support from the Natural Science Foundation(NSF) of China(Nos.22205015,22175020,and 22235001)the National Postdoctoral Program for Innovative Talents(No.BX20220032)+1 种基金the China Postdoctoral Science Foundation Funded Project(No.2022BG013)the Fundamental Research Funds for the Central Universities(Nos.00007709 and 00007770)。
文摘Dimensionality has great influence on the photo/electro-catalysts properties of covalent organic frameworks(COFs) because of the different electronic and porous structures.However,very rare attention has been paid on the dimensionality and function correlations of COF materials.In the present work,one new two-dimensional phthalocyanine COF,namely 2D-NiPc-COF,and one new three-dimensional phthalocyanine COF,namely 3D-NiPc-COF,were fabricated according to the imide reaction between tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(Ⅱ) with [2,2-bipyridine]-5,5-diamine and tetrakis(4-aminophenyl) methane,respectively.The crystalline structures of both COFs are verified by the powder X-ray diffraction analysis,computational simulation,and high resolution transmission electron microscopy measurement.Notably,3D-NiPc-COF with dispersed conjugated modules has high utilization efficiency of NiPc electroactive sites of 26.8%,almost two times higher than the in-plane stacking2D-NiPc-COF measured by electrochemical measurement,in turn resulting in its superior electrocatalytic performance with high CO_(2)-to-CO Faradaic efficiency over 90% in a wide potential window,a large partial CO current density of-13.97 mA/cm^(2) at-0.9 V(vs.reversible hydrogen electrode) to 2D-NiPc-COF.Moreover,3D-NiPc-COF has higher turnover number and turnover frequency of 5741.6 and 0.18 s^(-1) at-0.8 V during 8 h lasting measurement.The present work provides an example for the investigation on the correlation between dimensionality and electrochemical properties of 2D and 3D phthalocyanine COFs.
基金supported by the Young Scientist Funding(22409158,D.R.)from the National Natural Science Foundation of China。
文摘The increasing level of atmospheric carbon dioxide(CO_(2))caused by intensified human activities has exacerbated the greenhouse effect,calling for the technology of CO_(2)fixation.Among the proposed technologies,electrocatalytic CO_(2)reduction in acidic electrolytes has garnered significant attention for its potential in sustainable carbon utilization and renewable energy storage.This review provides a summary of recent advancements in acidic CO_(2)reduction,with a focus on catalyst design strategies,the optimization of the local reaction environment,and the effect of cations.We first evaluated the performance and discussed the challenges for acidic CO_(2)reduction in H-type cells,flow cells,and membrane electrode assembly.Afterward,we highlight the innovative strategies for promoting CO_(2)reduction through optimizing the intrinsic activity and regulating the local environment of catalysts.The critical role of cations in enhancing CO_(2)reduction selectivity is also discussed.The review concludes with an outlook on future research directions,especially the need for the design of catalysts and systems that are stable,scalable,and highly efficient.
基金Project supported by the National Key Research and Development Project of China(2022YFC2905202)Natural Science Foundation of Jiangxi Province(20232ACB204014)Youth Jinggang Scholars Program in Jiangxi Province(QNJG2019056)。
文摘The calcium-containing rare earth solution is generated during the recovery processes of NdFeB waste,which is treated as wastewater by enterprises.In this paper,the carbon dioxide carbonization method was applied to the separation of rare earths and calcium in the solution,as well as the preparation of rare earth oxides with a large specific surface.It is shown that the process of CO_(2)carbonization of solution includes reactions such as the dissolution,diffusion and ionization of CO_(2),the carbonate precipitation of rare earth ions,and the neutralization of hydrogen ions.At a pH of 4.5,the carbonization precipitation rate is effectively controlled,enabling homogeneous precipitation and ensuring both high precipitation yield and rare earth oxides purity.In this way,the crystallization of carbonization products is a process dominated by the oriented attachment theory and coexisting with the Ostwald ripening theory,resulting in abundant pores formed by multiple layers of stacking in the products.With the optimal carbonization conditions,the rare earth precipitation yield solution reaches 99.32%.The obtained carbonization products are crystalline(LaCe)(CO_(3))_(3)·8H_(2)O,and the purity of the rare earth oxides is as high as 99.22 wt%.The specific surface area of the rare earth oxides reaches 94.7 m^(2)/g,and its adsorption efficiency for tetracycline hydrochloride in solution can reach 92.6%in a short time.The rare earth oxides are expected to be used as an adsorption material for wastewater treatment and other adsorption environments.
文摘This study investigates the application of carbon dioxide (CO2) sequestration to address challenges in water-drive gas reservoirs, specifically focusing on improving gas recovery and mitigating water invasion. Traditional methods like blow-down and co-production have limitations, including sand production, water coning, and inefficiency in strong aquifers. To overcome these issues, this research explores CO2 injection near the edge aquifer, aiming to reduce water influx and enhance gas recovery through the propagation of a CO2 plume in the gas-water contact zone. Both synthetic and real compositional reservoir models were studied, with CO2 injection performed while maintaining reservoir pressure below 90% of the initial level. Results show that CO2 sequestration significantly improved recovery, particularly in higher permeability reservoirs, where it reduced aquifer influx and increased gas production by 26% under challenging conditions. While CO2 dissolution in water decreased aquifer influx by 39%, its adverse effect on sweep efficiency led to a reduction in gas and water production by 4.2% and 10%, respectively. The method's effectiveness was not significantly impacted by aquifer permeability, but it was sensitive to vertical-to-horizontal permeability ratios. When applied to a real gas reservoir, the proposed method increased gas production by 14% compared to conventional techniques, with minimal CO2 production over a 112-year period. This study demonstrates the potential of CO2 sequestration as a comprehensive solution for enhancing gas recovery, reducing water production, and mitigating environmental impacts in water-drive gas reservoirs.
