CAS-ESM2.0 Dataset for the Carbon Dioxide Removal Model Intercomparison Project(CDRMIP)

Understanding the response of the Earth system to varying concentrations of carbon dioxide(CO_(2))is critical for projecting possible future climate change and for providing insight into mitigation and adaptation strategies in the near future.In this study,we generate a dataset by conducting an experiment involving carbon dioxide removal(CDR)—a potential way to suppress global warming—using the Chinese Academy of Sciences Earth System Model version 2.0(CASESM2.0).A preliminary evaluation is provided.The model is integrated from 200–340 years as a 1%yr^(−1) CO_(2) concentration increase experiment,and then to~478 years as a carbon dioxide removal experiment until CO_(2) returns to its original value.Finally,another 80 years is integrated in which CO_(2) is kept constant.Changes in the 2-m temperature,precipitation,sea surface temperature,ocean temperature,Atlantic meridional overturning circulation(AMOC),and sea surface height are all analyzed.In the ramp-up period,the global mean 2-m temperature and precipitation both increase while the AMOC weakens.Values of all the above variables change in the opposite direction in the ramp-down period,with a delayed peak relative to the CO_(2) peak.After CO_(2) returns to its original value,the global mean 2-m temperature is still~1 K higher than in the original state,and precipitation is~0.07 mm d^(–1) higher.At the end of the simulation,there is a~0.5°C increase in ocean temperature and a 1 Sv weakening of the AMOC.Our model simulation produces similar results to those of comparable experiments previously reported in the literature.

Effects of drip and flood irrigation on carbon dioxide exchange and crop growth in the maize ecosystem in the Hetao Irrigation District,China

Drip irrigation and flood irrigation are major irrigation methods for maize crops in the Hetao Irrigation District,Inner Mongolia Autonomous Region,China.This research delves into the effects of these irrigation methods on carbon dioxide(CO_(2))exchange and crop growth in this region.The experimental site was divided into drip and flood irrigation zones.The irrigation schedules of this study aligned with the local commonly used irrigation schedule.We employed a developed chamber system to measure the diurnal CO_(2)exchange of maize plants during various growth stages under both drip and flood irrigation methods.From May to September in 2020 and 2021,two sets of repeated experiments were conducted.In each experiment,a total of nine measurements of CO_(2)exchange were performed to obtain carbon exchange data at different growth stages of maize crop.During each CO_(2)exchange measurement event,CO_(2)flux data were collected every two hours over a day-long period to capture the diurnal variations in CO_(2)exchange.During each CO_(2)exchange measurement event,the biological parameters(aboveground biomass and crop growth rate)of maize and environmental parameters(including air humidity,air temperature,precipitation,soil water content,and photosynthetically active radiation)were measured.The results indicated a V-shaped trend in net ecosystem CO_(2)exchange in daytime,reducing slowly at night,while the net assimilation rate(net primary productivity)exhibited a contrasting trend.Notably,compared with flood irrigation,drip irrigation demonstrated significantly higher average daily soil CO_(2)emission and greater average daily CO_(2)absorption by maize plants.Consequently,within the maize ecosystem,drip irrigation appeared more conducive to absorbing atmospheric CO_(2).Furthermore,drip irrigation demonstrated a faster crop growth rate and increased aboveground biomass compared with flood irrigation.A strong linear relationship existed between leaf area index and light utilization efficiency,irrespective of the irrigation method.Notably,drip irrigation displayed superior light use efficiency compared with flood irrigation.The final yield results corroborated these findings,indicating that drip irrigation yielded higher harvest index and overall yield than flood irrigation.The results of this study provide a basis for the selection of optimal irrigation methods commonly used in the Hetao Irrigation District.This research also serves as a reference for future irrigation studies that consider measurements of both carbon emissions and yield simultaneously.

Chemico-biological conversion of carbon dioxide

The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.

Solubility of iron(Ⅲ) and nickel(Ⅱ) acetylacetonates in supercritical carbon dioxide

As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.

Experimental investigation on the origin of carbonaceous materials in the fault zone of the Wenchuan earthquake

Carbonaceous materials in seismic fault zones may considerably influence seismic fault slip;however,the formation mechanism of carbonaceous materials remains unclear.In this study,we proposed a novel hypothesis for the formation of carbonaceous materials in fault gouge.Thus,we conducted a CO_(2) hydrogenation experiment in a high-temperature reactor at a co-seismic temperature,with fault gouge formed during the Wenchuan earthquake as the catalyst.Our experimental results demonstrate that carbonaceous materials in fault zones are formed on the fault gouge during the chemical reaction process,suggesting that the carbonaceous materials are possibly generated from the catalytic hydrogenation of CO_(2),followed by thermal cracking of its products.The results of this study provide a theoretical basis for understanding fault behavior and earthquake physics.

Criteria for Selecting Carbon Subsurface and Ocean Storage Site in Developing Countries: A Review

Important first phases in the process of implementing CO2 subsurface and ocean storage projects include selecting of best possible location(s) for CO2 storage, and site selection evaluation. Sites must fulfill a number of criteria that boil down to the following basics: they must be able to accept the desired volume of CO2 at the rate at which it is supplied from the CO2 source(s);they must as well be safe and reliable;and must comply with regulatory and other societal requirements. They also must have at least public acceptance and be based on sound financial analysis. Site geology;hydrogeological, pressure, and geothermal regimes;land features;location, climate, access, etc. can all be refined from these basic criteria. In addition to aiding in site selection, site characterization is essential for other purposes, such as foreseeing the fate and impacts of the injected CO2, and informing subsequent phases of site development, including design, permitting, operation, monitoring, and eventual abandonment. According to data from the IEA, in 2022, emissions from Africa and Asias emerging markets and developing economies, excluding Chinas, increased by 4.2%, which is equivalent to 206 million tonnes of CO2 and were higher than those from developed economies. Coal-fired power generation was responsible for more than half of the rise in emissions that were recorded in the region. The difficulty of achieving sustainable socio-economic progress in the developing countries is entwined with the work of reducing CO2 emissions, which is a demanding project for the economy. Organisations from developing countries, such as Bangladesh, Cameroon, India, and Nigeria, have formed partnerships with organisations in other countries for lessons learned and investment within the climate change arena. The basaltic rocks, coal seams, depleted oil and gas reservoirs, soils, deep saline aquifers, and sedimentary basins that developing countries (Bangladesh, Cameroon, India, and Nigeria etc.) possess all contribute to the individual countrys significant geological sequestration potential. There are limited or no carbon capture and storage or clean development mechanism projects running in these countries at this time. The site selection and characterization procedure are not complete without an estimate of the storage capacity of a storage location. Estimating storage capacity relies on volumetric estimates because a site must accept the planned volume of CO2 during the active injection period. As more and more applications make use of site characterization, so too does the body of written material on the topic. As the science of CO2 storage develops, regulatory requirements are implemented, field experience grows, and the economics of CO2 capture and storage improve, so too will site selection and characterisation change.

Efficient conversion of CO_(2) into cyclic carbonates under atmospheric by halogen and metal-free poly(ionic liquid)s

A novel series of halogen free, hydroxyl group containing poly(ionic liquid)s(PILs) was first synthesized from glycerol dimethyl acrylate(GDA) and 1-vinyl imidazole(1-VIM) through free radical polymerization, follow by an alkylation step and an ion-exchange procedure to form the final imidazolium hydrogen carbonate heterogenous catalyst poly(HCO_(3)-OH-n). The chemical and physical properties were investigated by varying the monomer ratio between GDA and 1-VIM. Among them, poly(HCO_(3)-OH-2) exhibited the highest catalytic activity for CO_(2)cycloaddition, with the yield of chloropropene carbonate 90% under mild conditions(80℃, 0.1 MPa, 12 h, 0.15 g catalyst for 32 mmol epichlorohydrin) in the absence of any cocatalyst, metal or solvent. A range of substrates with good to excellent yields under atmosphere was obtained. The poly(HCO_(3)-OH-n) catalyst is collectable and still remains acceptable catalytic activity after six runs. Finally, a preliminary kinetic is calculated on the basis of poly(HCO_(3)-OH-2) with the activation energy value of 79.5 kJ·mol^(-1). This study highlights that the poly(HCO_(3)-OH-n) enable to reach efficient CO_(2) conversion under mild conditions.

Progress, challenge and significance of building a carbon industry system in the context of carbon neutrality strategy

Carbon dioxide storage and utilization has become an inevitable trend and choice for sustainable development under the background of global climate change and carbon neutrality.Carbon industry which is dominated by CO_(2) capture,utilization and storage/CO_(2) capture and storage(CCUS/CCS)is becoming a new strategic industry under the goal of carbon neutrality.The sustainable development of carbon industry needs to learn from the experiences of global oil and gas industry development.There are three types of“carbon”in the earth system.Black carbon is the CO_(2) that has not been sequestered or used and remains in the atmosphere for a long time;grey carbon is the CO_(2) that has been fixed or permanently sequestered in the geological body,and blue carbon is the CO_(2) that could be converted into products for human use through biological,physical,chemical and other ways.The carbon industry system covers carbon generation,carbon capture,carbon transportation,carbon utilization,carbon sequestration,carbon products,carbon finance,and other businesses.It is a revolutionary industrial field to completely eliminate“black carbon”.The development of carbon industry technical system takes carbon emission reduction,zero carbon,negative carbon and carbon economy as the connotation,and the construction of a low-cost and energy-efficient carbon industry system based on CCUS/CCS are strategic measures to achieve the goal of carbon neutrality and clean energy utilization globally.This will promote the“four 80%s”transformation of China's energy supply,namely,to 2060,the percentage of zero-carbon new energy in the energy consumption will be over 80%and the CO_(2) emission will be decreased by 80%to ensure the carbon emission reduction of total 80×10^(8) t from the percentage of carbon-based fossil energy in the energy consumption of over 80%,and the percentage of CO_(2) emission from energy of over 80%in 2021.The carbon industry in China is facing three challenges,large CO_(2) emissions,high percentage of coal in energy consumption,and poor innovative system.Three strategic measures are proposed accordingly,including:(1)unswervingly develop carbon industrial system and ensure the achievement of carbon neutrality as scheduled by 2060;(2)vigorously develop new energy sources and promote a revolutionary transformation of China’s energy production and consumption structure;(3)accelerate the establishment of scientific and technological innovation system of the whole CO_(2) industry.It is of great significance for continuously optimization of ecological environment and construction of green earth and ecological earth to develop the carbon industry system,utilize clean energy,and achieve the strategic goal of global carbon neutrality.

Progress and prospect of carbon dioxide capture, utilization and storage in CNPC oilfields

The development history of carbon capture,utilization and storage for enhanced oil recovery(CCUS-EOR)in China is comprehensively reviewed,which consists of three stages:research and exploration,field test and industrial application.The breakthrough understanding of CO_(2) flooding mechanism and field practice in recent years and the corresponding supporting technical achievements of CCUS-EOR project are systematically described.The future development prospects are also pointed out.After nearly 60 years of exploration,the theory of CO_(2) flooding and storage suitable for continental sedimentary reservoirs in China has been innovatively developed.It is suggested that C7–C15 are also important components affecting miscibility of CO_(2) and crude oil.The mechanism of rapid recovery of formation energy by CO_(2) and significant improvement of block productivity and recovery factor has been verified in field tests.The CCUS-EOR reservoir engineering design technology for continental sedimentary reservoir is established.The technology of reservoir engineering parameter design and well spacing optimization has been developed,which focuses on maintaining miscibility to improve oil displacement efficiency and uniform displacement to improve sweep efficiency.The technology of CO_(2) capture,injection and production process,whole-system anticorrosion,storage monitoring and other whole-process supporting technologies have been initially formed.In order to realize the efficient utilization and permanent storage of CO_(2),it is necessary to take the oil reservoir in the oil-water transition zone into consideration,realize the large-scale CO_(2) flooding and storage in the area from single reservoir to the overall structural control system.The oil reservoir in the oil-water transition zone is developed by stable gravity flooding of injecting CO_(2) from structural highs.The research on the storage technology such as the conversion of residual oil and CO_(2) into methane needs to be carried out.

Pulsed electrolysis of carbon dioxide by large-scale solid oxide electrolytic cells for intermittent renewable energy storage

CO_(2) electrolysis with solid oxide electrolytic cells(SOECs)using intermittently available renewable energy has potential applications for carbon neutrality and energy storage.In this study,a pulsed current strategy is used to replicate intermittent energy availability,and the stability and conversion rate of the cyclic operation by a large-scale flat-tube SOEC are studied.One hundred cycles under pulsed current ranging from -100 to -300 mA/cm^(2) with a total operating time of about 800 h were carried out.The results show that after 100 cycles,the cell voltage attenuates by 0.041%/cycle in the high current stage of−300 mA/cm^(2),indicating that the lifetime of the cell can reach up to about 500 cycles.The total CO_(2) conversion rate reached 52%,which is close to the theoretical value of 54.3% at -300 mA/cm^(2),and the calculated efficiency approached 98.2%,assuming heat recycling.This study illustrates the significant advantages of SOEC in efficient electrochemical energy conversion,carbon emission mitigation,and seasonal energy storage.

Micro-interface enhanced mass transfer sodium carbonate absorption carbon dioxide reaction

Micro-interface intensified reactor(MIR)can be applied in series/parallel in the absorption of CO_(2)in industrial gases by Na_(2)CO_(3)due to the ability to produce large numbers of stable microbubbles.This work focuses on the variation pattern of mass transfer characteristics parameters of the reaction gas in Na_(2)CO_(3) solution under the influence of different solution properties and operating parameters in the reaction of CO_(2)absorption by Na2CO3.The mass transfer characteristics parameters include bubble Sauter mean diameter,gas holdup,interfacial area,liquid side mass transfer coefficient,and liquid side volume mass transfer coefficient kLa.The solution properties and operating parameters include Na2CO3 concentration(0.05–2.0 mol·L^(-1)),superficial gas velocity(0.00221–0.01989 m·s^(-1)),superficial liquid velocity(0.00332–0.02984 m·s^(-1)),and ionic strength(1.42456–1.59588 mol·kg^(-1)).And volumetric mass transfer coeffi-cients kLa and superficial reaction rates r of the MIR and the bubble column reactor are compared in the reaction of sodium carbonate absorption of carbon dioxide,and the former shows a greater improvement under different solution properties and operating parameters.The enhanced role of MIR in mass transfer in non-homogeneous reactions is verified and the feasibility of industrial practical applications of MIR is demonstrated.

Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO_(2)

Electrochemical CO_(2) reduction reaction(CO_(2) RR) has attracted growing attention in energy storage and sustainable production of fuels and chemicals. N-doped carbon materials are preferred metal-free electrocatalysts, but it remains one challenge to finely engineer the active sites and porosity. Herein, we demonstrated that ionic porous polyamides were a kind of versatile precursors to prepare functional carbon materials in a one-step pyrolysis process. The polyamide precursors allowed the maintenance of abundant N species at high temperatures. The existence of ionic moieties and large specific surface area of the precursors promoted the formation of larger porosity carbon with a large specific surface area and sufficient active graphitic-N species by controlling the pyrolysis temperature. The catalyst was highly selective in the CO_(2) RR to produce CO with a maximum Faraday efficiency above 99%, attributable to the improved mass transfer in a large porosity system. This work shows that ionic polyamides are promising carbon precursors for the fabrication of metal-free electrocatalysts for CO_(2) RR.

Effects of zinc on χ-Fe_(5)C_(2) for carbon dioxide hydrogenation to olefins:Insights from experimental and density function theory calculations

Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. Carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.

Current situation of carbon emissions and countermeasures in China's ironmaking industry

The iron and steel industry(ISI) involves high energy consumption and high pollution. ISI in China, a leading country in the ISI,consumed 15% of the country’s total energy and produced more than 50% of the global ISI’s carbon emissions. Therefore, in the context of global low-carbon economy and emission reduction requirements, low-carbon smelting technology in the ISI has attracted increasingly more attention in China. This review summarizes the current status of carbon emissions and energy consumption in China’s ISI and discusses the development status and prospects of low-carbon ironmaking technology. The main route to effectively reducing carbon emissions is to develop a gas-based direct reduction process and replace sintering with pelletizing, both of which focus on developing pelletizing technology. However,the challenge of pelletizing process development is to obtain high-quality iron concentrates. Consequently, the present paper also summarizes the development status of China’s mineral processing technology, including fine-grained mineral processing technology, magnetization roasting technology, and flotation collector application. This paper aims to provide a theoretical basis for the low-carbon development of China’s ISI in terms of a dressing–smelting combination.

Dual atomic catalysts from COF-derived carbon for CO_(2)RR by suppressing HER through synergistic effects

The electrochemical carbon dioxide reduction reaction(CO_(2)RR)for highvalue-added products is a promising strategy to tackle excessive CO_(2) emissions.However,the activity of and selectivity for catalysts for CO_(2)RR still need to be improved because of the competing reaction(hydrogen evolution reaction).In this study,for the first time,we have demonstrated dual atomic catalytic sites for CO_(2)RR from a core-shell hybrid of the covalent-organic framework and the metal-organic framework.Due to abundant dual atomic sites(with CoN_(4)O and ZnN_(4) of 2.47 and 11.05 wt.%,respectively)on hollow carbon,the catalyst promoted catalysis of CO_(2)RR,with the highest Faradic efficiency for CO of 92.6%at-0.8 V and a turnover frequency value of 1370.24 h^(-1) at-1.0 V.More importantly,the activity and selectivity of the catalyst were well retained for 30 h.The theoretical calculation further revealed that CoN_(4)O was the main site for CO_(2)RR,and the activity of and selectivity for Zn sites were also improved because of the synergetic roles.

Anti-Melanogenesis Activity of Supercritical Carbon Dioxide Extract from Perilla frutescens Seeds

Perilla frutescens seed (PFS) oil is reported to inhibit skin photoaging;however, its effect on melanogenesis has not yet been investigated. Herein, we tested the anti-melanogenesis activity of an oil-based extract from PFS with supercritical carbon dioxide (scCO2). In a cell culture system, B16 mouse melanoma cells were treated with the PFS scCO2 extract and other samples. The PFS scCO2 extract decreased melanin production by approximately 90% in B16 mouse melanoma cells without cytotoxicity at 100 μg/mL. This effect was greater than that of the well-known melanogenesis inhibitor, kojic acid. Although a hexane-extracted PFS oil and a squeezed PFS oil also decreased melanin production in the B16 cells, the inhibitory effect of the PFS scCO2 extract was higher than both of these. Chemical analysis of the PFS scCO2 extract and squeezed PFS oil showed that almost 90% of the components of both oils were α-linolenic acid, linoleic acid, and oleic acid. Furthermore, the ratio of those three fatty acids across both samples was almost the same. When the three fatty acids were mixed in the same ratio as in the PFS scCO2 extract, the IC50 of the mixture for melanin production in B16 melanoma cells was identical to that of the PFS scCO2 extract. However, the IC50 of the squeezed PFS oil was approximately 6.6 times higher than that of the mixture. Although those fatty acids are the main inhibitory ingredients against melanin production in all of the extracts, some factor(s) in the squeezed PFS reduce their affinity with the cells. These results indicated that the PFS scCO2 extract could be a superior melanogenesis inhibitor. Although its main ingredients are probably the same as those of the squeezed PFS oil, it is necessary to extract with scCO2 for stronger anti-melanogenesis activity.

Defect engineering of high-loading single-atom catalysts for electrochemical carbon dioxide reduction

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor selectivity and low current density due to its sluggish kinetics and multitudinous reaction pathways.Single-atom catalysts(SACs)demonstrate outstanding activity,excellent selectivity,and remarkable atom utilization efficiency,which give impetus to the search for electrocatalytic processes aiming at high selectivity.There appears significant activity in the development of efficient SACs for CO_(2)RR,while the density of the atomic sites remains a considerable barrier to be overcome.To construct high-metal-loading SACs,aggregation must be prevented,and thus novel strategies are required.The key to creating high-density atomically dispersed sites is designing enough anchoring sites,normally defects,to stabilize the highly mobile separated metal atoms.In this review,we summarized the advances in developing high-loading SACs through defect engineering,with a focus on the synthesis strategies to achieve high atomic site loading.Finally,the future opportunities and challenges for CO_(2)RR in the area of high-loading single-atom electrocatalysts are also discussed.

Reactive ball-milling synthesis of Co-Fe bimetallic catalyst for efficient hydrogenation of carbon dioxide to value-added hydrocarbons

Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.

The fate of carbon resulting from pore water exchange in a mangrove and Spartina alterniflora ecozone

Mangrove and salt-marsh wetlands are important coastal carbon sinks.In order to quantify carbon export via pore water exchange and to evaluate subsequent fate of the exported carbon,we carried out continuous observations in a mangrove-Spartina alterniflora ecozone in the Zhangjiang River Estuary,China.The carbon fluxes via pore water exchange were estimated using^(222)Rn and^(228)Ra as tracers to be(2.15±0.63)mol/(m^(2)∙d)for dissolved inorganic carbon(DIC)and(-0.008±0.07)mol/(m^(2)∙d)for dissolved organic carbon(DOC)in the wet season and(3.02±0.65)mol/(m^(2)∙d)for DIC and(-0.15±0.007)mol/(m^(2)∙d)for DOC in the dry season in the mangrove-dominated creek(M-creek),while(2.52±0.82)mol/(m^(2)∙d)for DIC and(0.02±0.09)mol/(m^(2)∙d)for DOC in the dry season in the S.alterniflora-dominated creek(SA-creek).The negative value means that pore water was a sink of DOC in the creek.The total carbon via pore water exchange in the tidal creeks in the mangroves accounted for 41%-55%of the net carbon fixed by mangrove vegetation and was 3-4 times as much as the soil carbon accretion in the mangroves.The exported carbon in the form of DIC contributed all of the carbon outwelling from the M-creek and 79%of the carbon outwelling from the SA-creek,implying effective fixation of carbon by the wetland ecosystem.Moreover,it resulted in 54%in the dry season,75%in the wet season of the carbon dioxide released from the M-creek to the atmosphere,and 84%of the release from the SA-creek.Therefore,quantification of pore water exchange and related soil carbon loss is essential to trace the fate of carbon fixed in intertidal wetlands.

Modulating Pd e_(g) orbital occupancy in Pd-Au metallic aerogels for efficient carbon dioxide reduction

The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the orbitals.Herein,we present a new strategy to modulate the e_(g) orbital occupancy of Pd by constructing composition-controllable Pd-Au metallic aerogels(MAs),optimizing the d-band center of Pd to achieve excellent performance for electrochemical carbon dioxide reduction reaction(CO_(2)RR).Specifically,Pd_(1)Au_(2) MAs achieve almost 100% Faraday efficiency(FE) of CO in the range of-0.40 to-0.80 V vs.reversible hydrogen electrode(RHE),as well as the long-term stability,being one of the best Pd-based materials for CO_(2)RR.The X-ray photoelectron spectroscopy(XPS) results and density functional theory(DFT) calculations demonstrate that the introduction of Au modulates the Pd e_(g) orbital occupancy,which significantly weakens *CO adsorption on Pd,reduces the CO_(2)RR energy barrier and consequently improves the electrocatalytic activity and stability for long-term applications.Our work highlights a new strategy for designing efficient electrocatalysts for CO_(2)RR and beyond.