Porous carbons are considered promising for CO2 capture due to their high-pressure capture performance, high chemical/ thermal stability, and low humidity sensitivity. But, their low-pressure capture performance, selectivity toward CO2 over N2, and adsorption kinetics need further improvement for practical applications. Herein, we report a novel dual-templating strategy based on molten salts (LiBr/KBr) and hydrogen-bonded triazine molecules (melamine–cyanuric acid complex, MCA) to prepare high-performance porous carbon adsorbents for low-pressure CO2. The comprehensive investigations of pore structure, microstructure, and chemical structure, as well as their correlation with CO2 capture performance, reveal that the dual template plays the role of porogen for multi-hierarchical porous structure based on supermicro-/micro-/meso-/ macro-pores and reactant for high N/O insertion into the carbon framework. Furthermore, they exert a synergistic but independent effect on the carbonization procedure of glucose, avoiding the counter-balance between porous structure and hetero-atom insertion. This enables the preferred formation of pyrrolic N/carboxylic acid functional groups and supermicropores of ~ 0.8 nm, while retaining the micro-/meso-/macro-pores (> 1 nm) more than 60% of the total pore volume. As a result, the dual-templated porous carbon adsorbent (MG-Br-600) simultaneously achieves a high CO2 capture capacity of 3.95 mmol g− 1 at 850 Torr and 0 °C, a CO2/ N2 (15:85) selectivity factor of 31 at 0 °C, and a high intra-particle diffusivity of 0.23 mmol g− 1 min− 0.5 without performance degradation over repeated use. With the molecular scale structure tunability and the large-scale production capability, the dual-templating strategy will offer versatile tools for designing high-performance carbon-based adsorbents for CO2 capture.
Here, we report the preparation of microporous-activated carbons from a Brazilian natural lignocellulosic agricultural waste, cupuassu shell, by pyrolysis at 500 ºC and KOH activation under different experimental conditions and their subsequent application as adsorbent for CO2 capture. The effect of the KOH:precursor ratio (wt/wt%) and the activation temperature on the porous texture of activated carbons have been studied. The values of specific surface area ranged from 1132 to 2486 m2/ g, and the overall micropore volume ranged from 0.73 to 1.02 cm3/ g. Carbons activated with 2:1 ratio of KOH and activation temperature of 700 ºC presented a CO2 adsorption at 1 bar of 7.8 and 4.4 mmol/g at 0 °C and 25 ºC, respectively. The isosteric heat of adsorption, Qst , was calculated for all samples by applying the Clausius–Clapeyron approach to CO2 adsorption isotherms at both temperatures. The values of CO2 adsorption capacities are among the highest reported in the literature, especially for activated carbons produced from biomass.
Removing CO2 gas to address the global climate crisis is one of the most urgent agendas. To improve the CO2 adsorption ability of activated carbon, nitrogen plasma surface treatment was conducted. The effect of nitrogen plasma treatment on the surface chemistry and pore geometry of activated carbon was extensively analyzed. The porosity and surface groups of the activated carbon varied with the plasma treatment time. By plasma treatment for a few minutes, the microporosity and surface functionality could be simultaneously controlled. The changed microporosity and nitrogen groups affected the CO2 adsorption capacity and CO2 adsorption selectivity over N2. This simultaneous surface etching and functionalization effect could be achieved with a short operating time and low energy consumption.
The electrochemical reduction of carbon dioxide (CO2) to value-added products is a remarkable approach for mitigating CO2 emissions caused by the excessive consumption of fossil fuels. However, achieving the electrocatalytic reduction of CO2 still faces some bottlenecks, including the large overpotential, undesirable selectivity, and slow electron transfer kinetics. Various electrocatalysts including metals, metals oxides, alloys, and single-atom catalysts have been widely researched to suppress HER performance, reduce overpotential and enhance the selectivity of CO2RR over the last few decades. Among them, single-atom catalysts (SACs) have attracted a great deal of interest because of their advantages over traditional electrocatalysts such as maximized atomic utilization, tunable coordination environments and unique electronic structures. Herein, we discuss the mechanisms involved in the electroreduction of CO2 to carbon monoxide (CO) and the fundamental concepts related to electrocatalysis. Then, we present an overview of recent advances in the design of high-performance noble and non-noble singleatom catalysts for the CO2 reduction reaction.
본 연구에서는 PEBAX 2533에 합성된 PEI-GO@ZIF-8의 함량을 달리 첨가하여 혼합막을 제조하고 N2와 CO2의 투과 특성을 연구하였다. PEBAX/PEI-GO@ZIF-8 혼합막의 N2 투과도는 PEI-GO@ZIF-8 함량이 증가함에 따라 감소하였고, CO2 투과도는 PEI-GO@ZIF-8 함량에 따라 다른 경향을 보였는데 순수 PEBAX 막에서 PEI-GO@ZIF-8 0.1 wt%까지 CO2 투과도는 증가하다가 그 이후의 함량에서는 감소하였다. PEI-GO@ZIF-8 0.1 wt% 혼합막은 CO2 투과도 221.9 Barrer, CO2/N2 선택도는 60.0으로, 제조된 혼합막들 중 CO2 투과도와 CO2/N2 선택도가 향상되어 가장 높은 투과 특성을 보였고 Robeson upper-bound에 도달하는 결과를 얻었다. 이는 충진물이 PEBAX 내에 고루 분산되면서 CO2와 친화적인 상호작용을 하는 GO의 -COOH, -O-, -OH 작용기와 PEI에 결합된 아민기 그리고 CO2에 대해 gate-opening 현상이 일어나는 ZIF-8의 영 향 때문이다.
Crassulacean acid metabolism (CAM) plants use surplus CO2 generated by cooling and heating at night when ventilation is not needed in a greenhouse. Schlumbergera truncata ‘Pink Dew’ is a multi–flowering cactus that needs more phylloclades for high–quality production. This study examined photosynthetic characteristics by the phylloclade levels of S. truncata in a growth chamber and a greenhouse for use of night CO2 enrichment. The CO2 uptake rate of the S. truncata’s top phylloclade in a growth chamber exhibited a C3 pattern, and the second phylloclade exhibited a C3 –CAM pattern. The CO2 uptake rate of the top phylloclade in a greenhouse showed a negative value both day and night, but those of the second phylloclade exhibited a CAM pattern. The stomatal conductance and water–use efficiency (WUE) of S. truncata at both the top and second phylloclades were higher in a growth chamber than in a greenhouse. The WUE of S. truncata in a growth chamber and a greenhouse was higher at the second phylloclade, which is a CAM pattern compared with those of the top phylloclade. The daily total net CO2 uptake of S. truncata was higher in a growth chamber than in a greenhouse. The daily total net CO2 uptake of S. truncata at the second phylloclade had the highest value of 155 mmol·m–2·d–1 in a growth chamber. The night total CO2 uptake of S. truncata at the second phylloclade was 3–fold higher in a growth chamber than in a greenhouse. S. truncata’s second phylloclade exhibited a CAM pattern that uptake CO2 at night, and the second phylloclade, was more mature than the top phylloclade. A multi–flowering cactus S. truncata ‘Pink Dew’ efficiently uptake night surplus CO2 in the proper environmental condition with matured phylloclade.
The conversion of CO2 into solar fuels by photocatalysis is a promising way to deal with the energy crisis and the greenhouse effect. The introduction of oxygen vacancy into semiconductor has been proved to be an effective strategy for enhancing CO2 photoreduction performance. Herein, TiO2- x nanostructures have been prepared by a simple solvothermal method and engineered by the reaction time. With the prolonging of reaction time, the oxygen vacancy signal gradually increases while the band gap becomes narrow for the as-synthesized TiO2- x nanostructures. The results show that the TiO2- x-6 h, TiO2- x-24 h, and TiO2- x-48 h samples have the main product of CH4 (more) and CO (less) for CO2 photoreduction. Among the three oxygen vacancy photocatalysts, the TiO2- x-24 h sample shows the highest CH4 generation rate of 41.8 μmol g− 1 h− 1. On the basis of photo/electrochemical measurements, the TiO2- x-24 h sample exhibits efficient electron–hole separation and charge transfer capabilities, thus allows much more electrons to participate in the reaction and finally promotes the photocatalytic CO2 reduction reaction. It further confirms that the optimization of oxygen vacancy concentration could facilitate the photoinduced charge separation and accordingly improve photocatalytic CO2 conversion.
The physiological characteristics, growth, and yield of each regional rice variety (‘Odaebyeo’, ‘Saechucheong’, ‘Ilmibyeo’) were investigated depending on the impact of changes in temperature and CO2 concentration. Experiments were conducted with a control group, which reflected atmospheric CO2 concentration and temperature, and treatment groups, in which the CO2 concentration and temperature were increased by 250 ppm and 2.0℃ from those in the control group. The results showed that the increase in CO2 concentration and temperature reduced the growth and yield of the rice ‘Odaebyeo’, but did not substantially change the productivity of the ‘Saechucheong’ and ‘Ilmibyeo’. The increase in CO2 concentration and temperature increased stomatal conductance and rate of transpiration of the ‘Odaebyeo’ variety, thereby decreasing its water use efficiency (WUE). In contrast, the increase in CO2 concentration and temperature increased the photosynthetic rate and WUE of the ‘Saechucheong’ and ‘Ilmibyeo’ varieties. The gradual change in climate is considered to directly affect growth and development of rice and diversely affect the productivity of each variety. Therefore, it is necessary to implement technological development, select regionally optimal rice varieties, develop new rice varieties, as well as conduct long-term monitoring of each rice variety for climate adaptation to counter global warming.
The biocarbon (SKPH) was obtained from Sargassum spp., and it was evaluated electrochemically as support for the CO2 reduction. The biocarbon was synthesized and activated with KOH, obtaining a high surface area (1600 m2 g− 1) due to the activation process. Graphitic carbon formation after pyrolysis was confirmed by Raman spectroscopy. The XRD results show that SKPH has an amorphous structure with peaks corresponding to typical amorphous carbonaceous materials. FTIR was used to determine the chemical structure of SKPH. The bands at 3426, 2981, 2851, and 1604 cm− 1 correspond to O–H, C-H, and C-O stretching vibrations, respectively. Then, it compares SKPH films with different carbon films using two electrolytic systems with and without charge transfer. The SKPH film showed a capacitive behavior in the KOH, H2SO4, and, KCl systems; in the acid medium, the presence of a redox couple associated with carbon functional groups was shown. Likewise, in the [Fe(CN)6]−3 and Cu(II) systems, the charge transfer process coupled with a capacitive behavior was described, and this effect is more noticeable in the [Fe(CN)6]−3 system. Electrodeposition of copper on SKPH film showed two stages Cu(NH 3)2+ 4 /Cu(NH 3)+ 2 and Cu(NH 3)+ 2 ∕Cu in ammonia media. Hydrogen formation and the activity of CO2 are observed on SKPH film and are favored by the carbon’s surface chemistry. Cu/SKPH electrocatalyst has a catalytic effect on electrochemical reduction of CO2 and inhibition of hydrogen formation. This study showed that the SKPH film electrode responds as a capacitive material that can be used as an electrode for energy storage or as metal support.