Metal‐Organic Frameworks for Carbon Dioxide Capture and Methane Storage

In the global transition to a sustainable low‐carbon economy, CO₂ capture and storage technology still plays a critical role for deep emission reduction, particularly for the stationary sources in power generation and industry. However, for small and mobile emission sources in transportation, CO₂ capture is not suitable and it is more practical to use relatively clean energy, such as natural gas. In these two low‐carbon energy technologies, designing highly selective sorbents is one of the key and most challenging steps. Toward this end, metal‐organic frameworks (MOFs) have received continuously intensive attention in the past decades for their highly porous and diversified structures. In this review, the recent progress in developing MOFs for selective CO₂ capture from post‐combustion flue gas and CH₄ storage for vehicle applications are summarized. For CO₂ capture, several promising strategies being used to improve CO₂ adsorption uptake at low pressures are highlighted and compared. In addition, the conventional and novel regeneration techniques for MOFs are also discussed. In the case of CH₄ storage, the flexible and rigid MOFs, whose CH₄ storage capacity is close to the target set by U.S. Department of Energy are particularly emphasized. Finally, the challenge of using MOFs for CH₄ storage is discussed.     

Environmental assessment of German electricity generation from coal-fired power plants with amine-based carbon capture

Background, aim, and scope  

One of the most important sources of global carbon dioxide emissions is the combustion of fossil fuels for power generation. Power plants contribute more than 40% of the worldwide anthropogenic CO₂ emissions. Therefore, the increased requirements for climate protection are a great challenge for the power producers. In this context a significant increase in power plant efficiency will contribute to reduce specific CO₂ emissions. Additionally, CO₂ capture and storage (CCS) is receiving considerable attention as a greenhouse gas (GHG) mitigation option. CCS allows continued use of fossil fuels with no or little CO₂ emissions given to the atmosphere. This could approve a moderate transition to a low-carbon energy generation over the next decades. Currently, R&D activities in the field of CCS are mainly concentrated on the development of capture techniques, the geological assessment of CO₂ storage reservoirs, and on economic aspects. Although first studies on material and energy flows caused by CCS are available, a broader environmental analysis is necessary to show the overall environmental impacts of CCS. The objectives in this paper are coal-based power plants with and without CO₂ capture via mono-ethanolamine (MEA) and the comparison of their environmental effects based on life cycle assessment methodology (LCA).     

Production,purification, and characterization of a fusion protein of carbonic anhydrase from Neisseria gonorrhoeae and cellulose binding domain from Clostridium thermocellum

Carbon dioxide capture technologies have the potential to become an important climate change mitigation option through sequestration of gaseous CO₂. A new concept for CO₂ capture involves use of immobilized carbonic anhydrase (CA) that catalyzes the reversible hydration of CO₂ to HCO₃^? and H⁺. Cost‐efficient production of the enzyme and an inexpensive immobilization system are critical for development of economically feasible CA‐based CO₂ capture processes. An artificial, bifunctional enzyme containing CA from Neisseria gonorrhoeae and a cellulose binding domain (CBD) from Clostridium thermocellum was constructed with a His₆ tag. The chimeric enzyme exhibited both CA activity and CBD binding affinity. This fusion enzyme is of particular interest due to its binding affinity for cellulose and retained CA activity, which could serve as the basis for improved technology to capture CO₂ from flue gasses. © 2009 American Institute of Chemical Engineers Biotechnol. Prog., 2009     

The role of bioenergy for global deep decarbonization: CO2 removal or low‐carbon energy?

Bioenergy is expected to have a prominent role in limiting global greenhouse emissions to meet the climate change target of the Paris Agreement. Many studies identify negative emissions from bioenergy generation with carbon capture and storage (BECCS) as its key contribution, but assume that no other CO₂ removal technologies are available. We use a global integrated assessment model, TIAM‐UCL, to investigate the role of bioenergy within the global energy system when direct air capture and afforestation are available as cost‐competitive alternatives to BECCS. We find that the presence of other CO₂ removal technologies does not reduce the pressure on biomass resources but changes the use of bioenergy for climate mitigation. While we confirm that when available BECCS offers cheaper decarbonization pathways, we also find that its use delays the phase‐out of unabated fossil fuels in industry and transport. Furthermore, it displaces renewable electricity generation, potentially increasing the likelihood of missing the Paris Agreement target. We found that the most cost‐effective solution is to invest in a basket of CO₂ removal technologies. However, if these technologies rely on CCS, then urgent action is required to ramp up the necessary infrastructure. We conclude that a sustainable biomass supply is critical for decarbonizing the global energy system. Since only a few world regions carry the burden of producing the biomass resource and store CO₂ in geological storage, adequate international collaboration, policies and standards will be needed to realize this resource while avoiding undesired land‐use change.     

Quantifying the global warming potential of CO2 emissions from wood fuels

Recent studies have introduced the metric GWP_bio, an indicator of the potential global warming impact of CO₂ emissions from biofuels. When a time horizon of 100 years was applied, the studies found the GWP_bio of bioenergy from slow‐growing forests to be significantly lower than the traditionally calculated GWP of CO₂ from fossil fuels. This result means that bioenergy is an attractive energy source from a climate mitigation perspective. The present paper provides an improved method for quantifying GWP_bio. The method is based on a model of a forest stand that includes basic dynamics and interactions of the forest's multiple carbon pools, including harvest residues, other dead organic matter, and soil carbon. Moreover, the baseline scenario (with no harvest) takes into account that a mature stand will usually continue to capture carbon if not harvested. With these methodological adjustments, the resulting GWP_bio estimates are found to be two to three times as high as the estimates of GWP_bio found in other studies, and also significantly higher than the GWP of fossil CO₂, when a 100‐year time horizon is applied. Hence, the climate impact per unit of CO₂ emitted seems to be even higher for the combustion of slow‐growing biomass than for the combustion of fossil carbon in a 100‐year time frame.     

微藻固定燃烧烟气中CO2 的研究进展

空气中CO2浓度升高导致的气候变暖问题已经成为全球性的环境、科学、政治、经济问题。近年来,对可用于直接固定工业废气尤其是燃烧烟气中CO2的捕捉和封存 (CCS) 技术进行了广泛的研究。在这些技术中,微藻生物固定CO2是一种具有大规模应用前景和经济上可行的CCS技术。以下从藻种的筛选、烟气条件对微藻固定CO2的影响、高效光生物反应器的开发和微藻产物的利用等方面对微藻生物固定烟气中CO2的现状和发展以及作者所在实验室在这一领域的研究情况进行了分析和总结,最后对其技术前景进行了展望,以期对微藻固定燃烧烟气中CO     

Can biomass supply meet the demands of bioenergy with carbon capture and storage (BECCS)?

To reach the reduced carbon emission targets proposed by the Paris agreement, one of the widely proposed decarbonizing strategies, referred to as negative emissions technologies (NETs), is the production and combustion of bioenergy crops in conjunction with carbon capture and storage (BECCS). However, concerns have been increasingly raised that relying on the potential of BECCS to achieve negative emissions could result in delayed reductions in gross CO₂ emissions, with consequent high risk of overshooting global temperature targets. We focus on two particular issues: the carbon efficiency and payback time of bioenergy use in BECCS and the potential constraints on the supply of bioenergy. The simplistic vision of BECCS is that 1 tonne of CO₂ captured in the growth of biomass equates to 1 tonne of CO₂ sequestered geologically, but this cannot be the case as CO₂ is emitted by variable amounts during the lifecycle from crop establishment to sequestration below ground in geological formations. The deployment of BECCS is ultimately reliant on the availability of sufficient, sustainably sourced, biomass. The two most important factors determining this supply are land availability and land productivity. The upper bounds of the area estimates required correspond to more than the world's harvested land for cereal production. To achieve these estimates of biomass availability requires the rapid evolution of a multitude of technological, social, political and economic factors. Here, we question whether, because of the limited sustainable supply of biomass, BECCS should continue to be considered the dominant NET in IPCC and other scenarios achieving the Paris targets, or should it be deemed no longer fit for purpose?     

Carbon Recycling for Renewable Materials and Energy Supply

The current flow of carbon for the production, use, and waste management of polymer‐based products is still mostly linear from the lithosphere to the atmosphere with rather low rates of material recycling. In view of a limited future supply of biomass, this article outlines the options to further develop carbon recycling (C‐REC). The focus is on carbon dioxide (CO₂) capture and use for synthesis of platform chemicals to produce polymers. CO₂ may be captured from exhaust gases after combustion or fermentation of waste in order to establish a C‐REC system within the technosphere. As a long‐term option, an external C‐REC system can be developed by capturing atmospheric CO₂. A central role may be expected from renewable methane (or synthetic natural gas), which is increasingly being used for storage and transport of energy, but may also be used for renewable carbon supply for chemistry. The energy input for the C‐REC processes can come from wind and solar systems, in particular, power for the production of hydrogen, which is combined with CO₂ to produce various hydrocarbons. Most of the technological components for the system already exist, and, first modules for renewable fuel and polymer production systems are underway in Germany. This article outlines how the system may further develop over the medium to long term, from a piggy‐back add‐on flow system toward a self‐carrying recycling system, which has the potential to provide the material and energy backbone of future societies. A critical bottleneck seems to be the capacity and costs of renewable energy supply, rather than the costs of carbon capture.     

Direct capture and conversion of CO2 from air by growing a cyanobacterial consortium at pH up to 11.2

Bioenergy with carbon capture and storage (BECCS) is recognized as a potential negative emission technology, needed to keep global warming within safe limits. With current technologies, large-scale implementation of BECCS would compromise food production. Bioenergy derived from phototrophic microorganisms, with direct capture of CO₂ from air, could overcome this challenge and become a sustainable way to realize BECCS. Here we present an alkaline capture and conversion system that combines high atmospheric CO₂ transfer rates with high and robust phototrophic biomass productivity (15.2 ± 1.0 g/m ²/d). The system is based on a cyanobacterial consortium, that grows at high alkalinity (0.5 mol/L) and a pH swing between 10.4 and 11.2 during growth and harvest cycles.     

A comparison of the global warming effects of wood fuels and fossil fuels taking albedo into account

Traditionally, wood fuels, like other bioenergy sources, have been considered carbon neutral because the amount of CO₂ released can be offset by CO₂ sequestration due to the regrowth of the biomass. Thus, until recently, most studies assigned a global warming potential (GWP) of zero to CO₂ generated by the combustion of biomass (biogenic CO₂). Moreover, emissions of biogenic CO₂ are usually not included in carbon tax and emissions trading schemes. However, there is now increasing awareness of the inadequacy of this way of treating bioenergy, especially bioenergy from boreal forests. Holtsmark (2014) recently quantified the GWP of biogenic CO₂ from slow‐growing forests (GWP_bio), finding it to be significantly higher than the GWP of fossil CO₂ when a 100 year time horizon was applied. Hence, the climate impact seems to be even higher for the combustion of slow‐growing biomass than for the combustion of fossil carbon in a 100 year timeframe. The present study extends the analysis of Holtsmark (2014) in three ways. First, it includes the cooling effects of increased surface reflectivity after harvest (albedo). Second, it includes a comparison with the potential warming impact of fossil fuels, taking the CO₂ emissions per unit of energy produced into account. Third, the study links the literature estimating GWP_bio and the literature dealing with the carbon debt, and model simulations estimating the payback time of the carbon debt are presented. The conclusion is that, also after these extensions of the analysis, bioenergy from slow‐growing forests usually has a larger climate impact in a 100 year timeframe than fossil oil and gas. Whether bioenergy performs better or worse than coal depends on a number of conditions.     

Environmental Damage Assessment of Carbon Capture and Storage

An end‐point life cycle impact assessment is used to evaluate the damages of electricity generation from fossil fuel‐based power plants with carbon dioxide capture and storage (CCS) technology. Pulverized coal (PC), integrated gasification combined cycle (IGCC), and natural gas combined cycle (NGCC) power plants are assessed for carbon dioxide (CO₂) capture, pipeline transport, and storage in a geological formation. Results show that the CCS systems reduce the climate change‐related damages but increase the damages from toxicity, acidification, eutrophication, and resource consumption. Based on the currently available damage calculation methods, it is concluded that the benefit of reducing damage from climate change is larger than the increases in other damage categories, such as health effects from particulates or toxic chemicals. CCS significantly reduces the overall environmental damage, with a net reduction of 60% to 70% in human health damage and 65% to 75% in ecosystem damage. Most of the damage is due to fuel production and combustion processes. The energy and infrastructure demands of CCS cause increases in the depletion of natural resources by 33% for PC, 19% for IGCC, and 18% for NGCC power plants, mostly due to increased fossil fuel consumption.     

Nanoporous Au Thin Films on Si Photoelectrodes for Selective and Efficient Photoelectrochemical CO2 Reduction

An Si photoelectrode with a nanoporous Au thin film for highly selective and efficient photoelectrochemical (PEC) CO₂ reduction reaction (CO₂RR) is presented. The nanoporous Au thin film is formed by electrochemical reduction of an anodized Au thin film. The electrochemical treatments of the Au thin film critically improve CO₂ reduction catalytic activity of Au catalysts and exhibit CO Faradaic efficiency of 96% at 480 mV of overpotential. To apply the electrochemical pretreatment of Au films for PEC CO₂RR, a new Si photoelectrode design with mesh‐type co‐catalysts independently wired at the front and the back of the photoelectrode is demonstrated. Due to the superior CO₂RR activity of the nanoporous Au mesh and high photovoltage from Si, the Si photoelectrode with the nanoporous Au thin film mesh shows conversion of CO₂ to CO with 91% Faradaic efficiency at positive potential than the CO₂/CO equilibrium potential.     

Carbon dioxide emission from bamboo culms

Bamboos are one of the fastest growing plants on Earth, and are widely considered to have high ability to capture and sequester atmospheric carbon, and consequently to mitigate climate change. We tested this hypothesis by measuring carbon dioxide (CO₂) emissions from bamboo culms and comparing them with their biomass sequestration potential. We analysed diurnal effluxes from Bambusa vulgaris culm surface and gas mixtures inside hollow sections of various bamboos using gas chromatography. Corresponding variations in gas pressure inside the bamboo section and culm surface temperature were measured. SEM micrographs of rhizome and bud portions of bamboo culms were also recorded. We found very high CO₂ effluxes from culm surface, nodes and buds of bamboos. Positive gas pressure and very high concentrations of CO₂ were observed inside hollow sections of bamboos. The CO₂ effluxes observed from bamboos were very high compared to their carbon sequestration potential. Our measurements suggest that bamboos are net emitters of CO₂ during their lifespan.     

Superior CO2 Adsorption Capacity on N‐doped,High‐Surface‐Area,Microporous Carbons Templated from Zeolite

Zeolite‐templated, high‐surface‐area, microporous, N‐doped carbons exhibit the highest CO₂ uptake capacity recorded to date for any carbon material and one of the highest for any inorganic or organic porous material of up to 6.9 mmol g^?1 at 273 K and ambient pressure and 4.4 mmol g^?1 at ambient temperature and pressure, along with an initial CO₂ adsorption energy of 36 kJ mol^?1 at lower coverage and 20 kJ mol^?1 at higher CO₂ coverage. Combined with their ease of preparation, excellent recyclability and regeneration stability, and high selectivity for CO₂, the N‐doped zeolite‐templated carbons are amongst the most promising solid‐state absorbents reported so far for CO₂ capture and storage.     

Managing for soil carbon sequestration: Let’s get realistic

Improved soil management is increasingly pursued to ensure food security for the world's rising global population, with the ancillary benefit of storing carbon in soils to lower the threat of climate change. While all increments to soil organic matter are laudable, we suggest caution in ascribing large, potential climate change mitigation to enhanced soil management. We find that the most promising techniques, including applications of biochar and enhanced silicate weathering, collectively are not likely to balance more than 5% of annual emissions of CO₂ from fossil fuel combustion.     

Predicting long‐term carbon mineralization and trace gas production from thawing permafrost of Northeast Siberia

The currently observed Arctic warming will increase permafrost degradation followed by mineralization of formerly frozen organic matter to carbon dioxide (CO₂) and methane (CH₄). Despite increasing awareness of permafrost carbon vulnerability, the potential long‐term formation of trace gases from thawing permafrost remains unclear. The objective of the current study is to quantify the potential long‐term release of trace gases from permafrost organic matter. Therefore, Holocene and Pleistocene permafrost deposits were sampled in the Lena River Delta, Northeast Siberia. The sampled permafrost contained between 0.6% and 12.4% organic carbon. CO₂ and CH₄ production was measured for 1200 days in aerobic and anaerobic incubations at 4 °C. The derived fluxes were used to estimate parameters of a two pool carbon degradation model. Total CO₂ production was similar in Holocene permafrost (1.3 ± 0.8 mg CO₂‐C gdw^?1 aerobically, 0.25 ± 0.13 mg CO₂‐C gdw^?1 anaerobically) as in 34 000–42 000‐year‐old Pleistocene permafrost (1.6 ± 1.2 mg CO₂‐C gdw^?1 aerobically, 0.26 ± 0.10 mg CO₂‐C gdw^?1 anaerobically). The main predictor for carbon mineralization was the content of organic matter. Anaerobic conditions strongly reduced carbon mineralization since only 25% of aerobically mineralized carbon was released as CO₂ and CH₄ in the absence of oxygen. CH₄ production was low or absent in most of the Pleistocene permafrost and always started after a significant delay. After 1200 days on average 3.1% of initial carbon was mineralized to CO₂ under aerobic conditions while without oxygen 0.55% were released as CO₂ and 0.28% as CH₄. The calibrated carbon degradation model predicted cumulative CO₂ production over a period of 100 years accounting for 15.1% (aerobic) and 1.8% (anaerobic) of initial organic carbon, which is significantly less than recent estimates. The multiyear time series from the incubation experiments helps to more reliably constrain projections of future trace gas fluxes from thawing permafrost landscapes.     

Time‐dependent climate impact of a bioenergy system – methodology development and application to Swedish conditions

The area of dedicated energy crops is expected to increase in Sweden. This will result in direct land use changes, which may affect the carbon stocks in soil and biomass, as well as yield levels and the use of inputs. Carbon dioxide (CO₂) fluxes of biomass are often not considered when calculating the climate impact in life cycle assessments (LCA) assuming that the CO₂ released at combustion has recently been captured by the biomass in question. With the extended time lag between capture and release of CO₂ inherent in many perennial bioenergy systems, the relation between carbon neutrality and climate neutrality may be questioned. In this paper, previously published methodologies and models are combined in a methodological framework that can assist LCA practitioners in interpreting the time‐dependent climate impact of a bioenergy system. The treatment of carbon differs from conventional LCA practice in that no distinction is made between fossil and biogenic carbon. A time‐dependent indicator is used to enable a representation of the climate impact that is not dependent on the choice of a specific characterization time horizon or time of evaluation and that does not use characterization factors, such as global warming potential and global temperature potential. The indicator used to aid in the interpretation phase of this paper is global mean surface temperature change (ΔT_s(n)). A theoretical system producing willow for district heating was used to study land use change effects depending on previous land use and variations in the standing biomass carbon stocks. When replacing annual crops with willow this system presented a cooling contribution to ΔT_s(n). However, the first years after establishing the willow plantation it presented a warming contribution to ΔT_s(n). This behavior was due mainly to soil organic carbon (SOC) variation. A rapid initial increase in standing biomass counteracted the initial SOC loss.     

Carbon dioxide capture by planar (AlN)<Subscript>n</Subscript> clusters (<Emphasis Type="Italic">n</Emphasis>=3–5)

Searching for materials and technologies of efficient CO₂ capture is of the utmost importance to reduce the CO₂ impact on the environment. Therefore, the (AlN)_n clusters (n = 3–5) are researched using density functional theoretical calculations. The results of the optimization show that the most stable structures of (AlN)_n clusters all display planar configurations at B3LYP and G3B3 methods, which are consistent with the reported results. For these planar clusters, we further systematically studied their interactions with carbon dioxide molecules to understand their adsorption behavior at the B3LYP/6–311+G(d,p) level, including geometric optimization, binding energy, bond index, and electrostatic. We found that the planar structures of (AlN)_n (n = 3–5) can capture 3–5 CO₂ molecules. The result indicates that (AlN)_n (n = 3–5) clusters binding with CO₂ is an exothermic process (the capture of every CO₂ molecule on (AlN)_n clusters releases at least 30 kcal mol^-1 in relative free energy values). These analysis results are expected to further motivate the applications of clusters to be efficient CO₂ capture materials.