Cu/TiO_(2) Photocatalysts for CO_(2) Reduction: Structure and Evolution of the Cocatalyst Active Form

Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spectroscopy, high-resolution transmis- sion electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. It was found that copper exists in different states (Cu 0 , Cu^(+) , and Cu^(2+) ), the content of which depends on the TiO_(2) calcination temperature and copper loading. The optimum composition of the cocatalyst has a photocatalyst based on TiO_(2) calcined at 700℃ and modified with 5 wt% copper, the activity of which is 22 μmol/(h·g cat ) (409 nm). Analysis of the photocatalysts after the photocatalytic reaction disclosed that the copper metal on the surface of the calcined TiO_(2) was gradually converted into Cu_(2) O during the photocatalytic reaction. Meanwhile, the metallic copper on the surface of the noncalcined TiO_(2) did not undergo any trans- formation during the reaction.

Low-energy-consumption temperature swing system for CO_(2) capture by combining passive radiative cooling and solar heating

Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.

The photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)for stable photocatalytic CO_(2)reduction

Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.

Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO_(2) Reduction

We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.

Mechanistic investigation on Ag-Cu_(2)O in electrocatalytic CO_(2) to CH_(4) by in situ/operando spectroscopic and theoretical analysis

Silver-copper electrocatalysts have demonstrated effectively catalytic performance in electroreduction CO_(2) toward CH_(4),yet a revealing insight into the reaction pathway and mechanism has remained elusive.Herein,we construct chemically bonded Ag-Cu_(2)O boundaries,in which the complete reduction of Cu_(2)O to Cu has been strongly impeded owing to the presence of surface Ag shell.The interfacial confinement effect helps to maintain Cu^(+)sites at the Ag-Cu_(2)O boundaries.Using in situ/operando spectroscopy and theoretical simulations,it is revealed that CO_(2) is enriched at the Ag-Cu_(2)O boundaries due to the enhanced physisorption and chemisorption to CO_(2),activating CO_(2) to form the stable intermediate^(*)CO.The boundaries between Ag shell and the Cu_(2)O mediate local^(*)CO coverage and promote^(*)CHO intermediate formation,consequently facilitating CO_(2)-to-CH_(4) conversion.This work not only reveals the structure-activity relationships but also offers insights into the reaction mechanism on Ag-Cu catalysts for efficient electrocatalytic CO_(2) reduction.

Cu-Based Materials for Enhanced C_(2+) Product Selectivity in Photo-/Electro-Catalytic CO_(2) Reduction: Challenges and Prospects

Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.

Multi-objective optimization and evaluation of supercritical CO_(2) Brayton cycle for nuclear power generation

The supercritical CO_(2) Brayton cycle is considered a promising energy conversion system for Generation IV reactors for its simple layout,compact structure,and high cycle efficiency.Mathematical models of four Brayton cycle layouts are developed in this study for different reactors to reduce the cost and increase the thermohydraulic performance of nuclear power generation to promote the commercialization of nuclear energy.Parametric analysis,multi-objective optimizations,and four decision-making methods are applied to obtain each Brayton scheme’s optimal thermohydraulic and economic indexes.Results show that for the same design thermal power scale of reactors,the higher the core’s exit temperature,the better the Brayton cycle’s thermo-economic performance.Among the four-cycle layouts,the recompression cycle(RC)has the best overall performance,followed by the simple recuperation cycle(SR)and the intercooling cycle(IC),and the worst is the reheating cycle(RH).However,RH has the lowest total cost of investment(C_(tot))of$1619.85 million,and IC has the lowest levelized cost of energy(LCOE)of 0.012$/(kWh).The nuclear Brayton cycle system’s overall performance has been improved due to optimization.The performance of the molten salt reactor combined with the intercooling cycle(MSR-IC)scheme has the greatest improvement,with the net output power(W_(net)),thermal efficiencyη_(t),and exergy efficiency(η_(e))improved by 8.58%,8.58%,and 11.21%,respectively.The performance of the lead-cooled fast reactor combined with the simple recuperation cycle scheme was optimized to increase C_(tot) by 27.78%.In comparison,the internal rate of return(IRR)increased by only 7.8%,which is not friendly to investors with limited funds.For the nuclear Brayton cycle,the molten salt reactor combined with the recompression cycle scheme should receive priority,and the gas-cooled fast reactor combined with the reheating cycle scheme should be considered carefully.

Boosting oxygen reduction activity and CO_(2) resistance on bismuth ferrite-based perovskite cathode for low-temperature solid oxide fuel cells below 600℃

Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.

Engineering of oxygen vacancy and bismuth cluster assisted ultrathin Bi_(12)O_(17)Cl_(2)nanosheets with efficient and selective photoreduction of CO_(2)to CO

The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.

High-efficiency sodium storage of Co_(0.85)Se/WSe_(2) encapsulated in N-doped carbon polyhedron via vacancy and heterojunction engineering

With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+adsorption.However,their synchronous engineering is rarely reported.Herein,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization strategy.Spherical aberration-corrected transmission electron microscopy confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se vacancies.Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,respectively.As expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1) at 20 A g^(−1)),outperforming almost all Co/W-based selenides.

Construction and Application of a Regional Kilometer-Scale Carbon Source and Sink Assimilation Inversion System(CCMVS-R)

CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.

In-situ coating and surface partial protonation co-promoting performance of single-crystal nickel-rich cathode in all-solid-state batteries

The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poor crystal structure stability of Ni-rich cathode.Several coating strategies are previously employed to enhance the stability of the cathodic interface and crystal structure for Ni-rich cathode.However,these methods can hardly achieve simplicity and high efficiency simultaneously.In this work,polyacrylic acid(PAA)replaced traditional PVDF as a binder for cathode,which can achieve a uniform PAA-Li(LixPAA(0<x≤1))coating layer on the surface of single-crystal LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)due to H^(+)/Li^(+)exchange reaction during the initial charging-discharging process.The formation of PAA-Li coating layer on cathode can promote interfacial Li^(+)transport and enhance the stability of the cathodic interface.Furthermore,the partially-protonated surface of SC-NCM83 casued by H^(+)/Li^(+)exchange reaction can restrict Ni ions transport to enhance the crystal structure stability.The proposed SC-NCM83-PAA exhibits superior cycling performance with a retention of 92%compared with that(57.3%)of SC-NCM83-polyvinylidene difluoride(PVDF)after 200 cycles.This work provides a practical strategy to construct high-performance cathodes for ASSBs.

A review of interaction mechanisms and microscopic simulation methods for CO_(2)-water-rock system

This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscopic simulations of CO_(2)-water-rock system.The work points out the key issues in current research and provides suggestions for future research.After injection of CO_(2) into underground reservoirs,not only conventional pressure-driven flow and mass transfer processes occur,but also special physicochemical phenomena like dissolution,precipitation,and precipitate migration.The coupling of these processes causes complex changes in permeability and porosity parameters of the porous media.Pore-scale microscopic flow simulations can provide detailed information within the three-dimensional pore and throat space and explicitly observe changes in the fluid-solid interfaces of porous media during reactions.At present,the research has limitations in the decoupling of complex mechanisms,characterization of differential multi-mineral reactions,precipitation generation mechanisms and characterization(crystal nucleation and mineral detachment),simulation methods for precipitation-fluid interaction,and coupling mechanisms of multiple physicochemical processes.In future studies,it is essential to innovate experimental methods to decouple“dissolution-precipitation-precipitate migration”processes,improve the accuracy of experimental testing of minerals geochemical reaction-related parameters,build reliable characterization of various precipitation types,establish precipitation-fluid interaction simulation methods,coordinate the boundary conditions of different physicochemical processes,and,finally,achieve coupled flow simulation of“dissolution-precipitation-precipitate migration”within CO_(2)-water-rock systems.

An integrated technology for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment

In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are investigated.The results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)absorption.The absorption rate and amount of CO_(2)under high gravity are higher than that under normal gravity.Notably,the absorption rate at 75 min under high gravity is approximately 2 times that under normal gravity.This is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and micromixing.The particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.

Impacts of forest plantation programs on sectoral CO_(2) emissions regionally in New Zealand

Investing in projects that support environmental benefits,such as tree harvesting,has the potential to reduce air pollution levels in the atmosphere in the future.However,this kind of investment may increase the current level of emissions.Therefore,it is necessary to estimate how much the policy affects the current level of CO_(2) emissions.This makes sure the policy doesn’t increase the level of CO_(2) emis-sions.This study aims to analyze the effect of the One Bil-lion Trees program on CO_(2) emissions in New Zealand by employing the 2020 input–output table analysis.This inves-tigation examines the direct and indirect effects of policy on both the demand and supply sides across six regions of New Zealand.The results of this study for the first year of plantation suggest that the policy increases the level of CO_(2) emissions in all regions,especially in the Waikato region.The direct and indirect impact of the policy leads to 64 kt of CO_(2) emissions on the demand side and 270 kt of CO_(2) emis-sions on the supply side.These lead to 0.19 and 0.74%of total CO_(2) emissions being attributed to investment shocks.Continuing the policy is recommended,as it has a low effect on CO_(2) emissions.However,it is crucial to prioritize the use of low-carbon machinery that uses fossil fuels during the plantation process.

Assessing the Viability of Gandhar Field in India’s Cambay Basin for CO_(2) Storage

Our research is centered on the Gandhar oil field, which was discovered in 1983, where daily oil production has declined significantly over the years. The primary objective was to evaluate the feasibility of carbon dioxide(CO_(2)) storage through its injection into the siliciclastic reservoirs of Ankleshwar Formation. We aimed to obtain high-resolution acoustic impedance data to estimate porosity employing model-based poststack seismic inversion. We conducted an analysis of the density and effective porosity in the target zone through geostatistical techniques and probabilistic neural networks. Simultaneously, the work also involved geomechanical analysis through the computation of pore pressure and fracture gradient using well-log data, geological information, and drilling events in the Gandhar field. Our investigation unveiled spatial variations in effective porosity within the Hazad Member of the Ankleshwar Formation, with an effective porosity exceeding 25% observed in several areas, which indicates the presence of well-connected pore spaces conducive to efficient CO_(2) migration. Geomechanical analysis showed that the vertical stress(Sv) ranged from 55 MPa to 57 MPa in Telwa and from 63.7 MPa to 67.7 MPa in Hazad Member. The pore pressure profile displayed variations along the stratigraphic sequence, with the shale zone, particularly in the Kanwa Formation, attaining the maximum pressure gradient(approximately 36 MPa). However, consistently low pore pressure values(30-34 MPa) considerably below the fracture gradient curves were observed in Hazad Member due to depletion. The results from our analysis provide valuable insights into shaping future field development strategies and exploration of the feasibility of CO_(2) sequestration in Gandhar Field.

Geochemical modeling to aid experimental design for multiple isotope tracer studies of coupled dissolution and precipitation reaction kinetics

It is a challenge to make thorough but efficient experimental designs for the coupled mineral dissolution and precipitation studies in a multi-mineral system, because it is difficult to speculate the best experimental duration, optimal sampling schedule, effects of different experimental conditions, and how to maximize the experimental outputs prior to the actual experiments. Geochemical modeling is an efficient and effective tool to assist the experimental design by virtually running all scenarios of interest for the studied system and predicting the experimental outcomes. Here we demonstrated an example of geochemical modeling assisted experimental design of coupled labradorite dissolution and calcite and clayey mineral precipitation using multiple isotope tracers. In this study, labradorite(plagioclase) was chosen as the reactant because it is both a major component and one of the most reactive minerals in basalt. Following our isotope doping studies of single minerals in the last ten years, initial solutions in the simulations were doped withmultiple isotopes(e.g., Ca and Si). Geochemical modeling results show that the use of isotope tracers gives us orders of magnitude more sensitivity than the conventional method based on concentrations and allows us to decouple dissolution and precipitation reactions at near-equilibrium condition. The simulations suggest that the precise unidirectional dissolution rates can inform us which rate laws plagioclase dissolution has followed. Calcite precipitation occurred at near-equilibrium and the multiple isotope tracer experiments would provide near-equilibrium precipitation rates, which was a challenge for the conventional concentration-based experiments. In addition, whether the precipitation of clayey phases is the rate-limiting step in some multi-mineral systems will be revealed. Overall, the modeling results of multimineral reaction kinetics will improve the understanding of the coupled dissolution–precipitation in the multi-mineral systems and the quality of geochemical modeling prediction of CO_(2) removal and storage efficacy in the basalt systems.

Continuous-flow electrosynthesis of urea and oxalic acid by CO_(2)-nitrate reduction and glycerol oxidation

Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.

Recent advances in intermediate-temperature CO_(2) capture: Materials,technologies and applications

Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate change.Among various CO_(2) adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen utilization,specifically in the water gas shift,steam reforming and gasification processes.These processes are crucial for achieving carbon neutrality.While laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial environments remains challenging,impeding the commercialization process.This review aims to critically summarize the recent research progress made in intermediatetemperature(200-400℃) solid CO_(2) adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application scenarios.Additionally,we provide an overview of laboratory-level advanced technologies specifically tailored for industrial applications.Furthermore,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale implementation.The insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial applications.By promoting advances in the application of solid adsorbents,we strive to facilitate the ultimate goal of achieving carbon neutrality.

A multi-mechanism numerical simulation model for CO_(2)-EOR and storage in fractured shale oil reservoirs

Under the policy background and advocacy of carbon capture,utilization,and storage(CCUS),CO_(2)-EOR has become a promising direction in the shale oil reservoir industry.The multi-scale pore structure distribution and fracture structure lead to complex multiphase flow,comprehensively considering multiple mechanisms is crucial for development and CO_(2) storage in fractured shale reservoirs.In this paper,a multi-mechanism coupled model is developed by MATLAB.Compared to the traditional Eclipse300 and MATLAB Reservoir Simulation Toolbox(MRST),this model considers the impact of pore structure on fluid phase behavior by the modified Peng—Robinson equation of state(PR-EOS),and the effect simultaneously radiate to Maxwell—Stefan(M—S)diffusion,stress sensitivity,the nano-confinement(NC)effect.Moreover,a modified embedded discrete fracture model(EDFM)is used to model the complex fractures,which optimizes connection types and half-transmissibility calculation approaches between non-neighboring connections(NNCs).The full implicit equation adopts the finite volume method(FVM)and Newton—Raphson iteration for discretization and solution.The model verification with the Eclipse300 and MRST is satisfactory.The results show that the interaction between the mechanisms significantly affects the production performance and storage characteristics.The effect of molecular diffusion may be overestimated in oil-dominated(liquid-dominated)shale reservoirs.The well spacing and injection gas rate are the most crucial factors affecting the production by sensitivity analysis.Moreover,the potential gas invasion risk is mentioned.This model provides a reliable theoretical basis for CO_(2)-EOR and sequestration in shale oil reservoirs.