FUEL
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2023
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IF 7.4
Miaomiao Tan,Xiangyu Li,Yu Feng,Bing Wang,Lina Han,Weiren Bao,Liping Chang,Jiancheng Wang
The ordered mesoporous silica materials with large pore volume were prepared from the silica source extracted from fly ash by supercritical hydrothermal activation. This path has the advantages of low activation temperature, high silicon utilization, and matching of silicon source extraction and the hydrothermal synthesis process. The obtained mesoporous silica support was impregnated with 60 wt% tetraethylenepentamine (TEPA) to prepare excellent solid amine sorbent. The thermogravimetric results showed that the CO 2 adsorption capacity of sorbent could reach 5.17 mmol/g under 75 °C and dry pure CO 2 atmosphere. At the same time, the sorbent had fast adsorption kinetics (5.08 mmol/g in 10 min) and stable cycle performance. Consequently, the obtained sorbent is a promising candidate for carbon capture technologies.
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CHEMBIOCHEM
·
2023
·Vol. 24
·期 10
·e202300114
·
IF 3.2
Bo-Yu Zhang,Zhen-Hua Wu,Zi-Yi Chu,Ke Li,Jia-Fu Shi
Graphical A monolithic catalyst of Filler-CA@Lys-HOF-1 (FCLH) was prepared by coating chemical sorption of CA on the surface of the filler followed by the coating of Lys-HOF-1. The highest catalytic activity of FCLH was obtained by regulating the amount of HOF-1 monomer added. Due to the protection of Lys-HOF-1, the FCLH showed good tolerance against acidity and salinity, which could retain about 80.2 % of the original activity after 9 h incubation in simulated seawater. The catalytic activity of FCLH could retain 85.4 % of the initial activity after 10 cycles. In short, we may offer a promising biocatalyst for carbon mineralization, which may drive down carbon emissions when used for CO 2 capture and conversion on offshore platforms. Exhausted emission of carbon dioxide (CO 2 ) from ships or offshore platforms has become one of the major contributors to global carbon emissions. Enzymes such as carbonic anhydrase (CA) have been widely used for CO 2 mineralization because of their high catalytic rate. However, CA in seawater is easy to inactivate and difficult to reuse. Immobilization would be a feasible solution to address the stability issue, which, however, may cause an increase of internal diffusion resistance and reduced catalytic activity. In this regard, design of high-performance biocatalysts for acquiring high catalytic activity and stability of CA is highly desirable. Herein, a monolithic catalyst of Filler-CA@Lys-HOF-1 (FCLH) was prepared by chemical sorption of CA on the surface of the Filler followed by the coating of Lys-HOF-1. The highest catalytic activity of FCLH was obtained by regulating the amount of HOF-1 monomer added. Due to the protection of Lys-HOF-1, the FCLH showed good tolerance against acidity and salinity, which could retain about 80.2 % of the original activity after 9 h incubation in simulated seawater. The catalytic activity of FCLH could retain 85.4 % of the initial activity after 10 cycles. Hopefully, our study can provide a promising biocatalyst for CO 2 mineralization, which may drive down carbon emissions when used for CO 2 capture and conversion on offshore platforms.
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Changcheng Wei,Wenna Zhang,Kuo Yang,Xiu Bai,Shutao Xu,Jinzhe Li,Zhongmin Liu
ABSTRACT The most promising method to eliminate CO 2 is to find large-scale and value-added applications of CO 2 as a carbon resource. However, the utilization of CO 2 as feedstock for basic chemicals has long been a great challenge owing to its high thermodynamic stability. Herein, we report the coupling conversion of CO 2 with light alkanes over the HZSM-5 zeolite with much higher aromatic selectivity than light alkanes as the only reactant. A CO 2 conversion of 17.5% and n -butane conversion of 100% with aromatic selectivity of 80% could be achieved by the coupling reaction at the CO 2 to n -butane ratio of 0.475, in which CO 2 not only acted as an agent for balancing hydrogen in the reaction but also partly (~25%) incorporated into the aromatic products. Methyl-substituted lactones (MLTOs) and methyl-substituted cycloalkenones (MCEOs) were identified as key intermediates during the coupling reaction. 13 C isotope labeling experiments, 13 C solid-state NMR, in-situ diffuse reflectance infrared Fourier transform spectroscopy, and density functional theory (DFT)calculations revealed that CO 2 could react with carbonium ions generated from alkane cracking to form MLTOs, which could further get converted into MCEOs, thus generating aromatic compounds . This coupling reaction provides guidance for the direct utilization of CO 2 to produce value-added chemicals with the simultaneous transformation of light alkanes.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Min Wang,Zhancheng Zhang,Tanju Yildirim,Libei Feng,Linglong Zhang,Jue Wang
Renewable electricity powered CO 2 electroreduction to methane is promising for producing highly specific combustion fuels. However, the reduction process is severely limited by poor selectivity and chemical activity at high electrolysis reaction rates. Herein, we produce tandem electrocatalysts by combining organic small molecules (perylene-3,4,9,10-tetracarboxylic dianhydride and pentacene) with copper catalysts supported on microporous polytetra fluoroethylene with enhanced *CO protonation and weakened hydrogen evolution. Experimental results show that the tandem catalysts effectively suppress the two-electron reduction process associated with hydrogen (H 2 ) and carbon monoxide (CO) production while inhibiting the multielectron conversion process associated with ethylene production (C 2 H 4 ). As a result, the tandem catalysts enable an efficient eight-electron transfer for electrochemical reduction of CO 2 and demonstrate a ∼ 50 % (±2%) Faradaic efficiency for CO 2 -to-methane conversion at a partial current density of 220 mA cm −2 in 1 M KHCO 3 solution. Notably, the selectively of CO 2 -to-CH 4 is 2.7 times higher than that of a copper catalyst supported on microporous polytetra fluoroethylene which is known to produce C 2 H 4 with ∼ 50 % Faradaic efficiency. This work paves the way for tuning *CO dimerization and hydrogen evolution reaction to maximize CO 2 methanation by using abundant organic molecular materials.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2022
·
IF 0.847
Zheyue Li,Di Wu,Wanbing Gong,Jiayi Li,Shuaikang Sang,Hengjie Liu,Ran Long,Yujie Xiong
Solar-driven CO 2 methanation is an imperative and promising approach to relieve the global warming and environmental crisis, yet remains a great challenge due to the low reaction efficiency, unsatisfactory selectivity and poor stability. In this work, we demonstrate a facile and efficient strategy to prepare Ru-doped TiO 2 photocatalyst with tunable oxygen vacancies using the ascorbic acid as a reducing agent for the CO 2 methanation reaction. The optimal Ru-TiO 2 -OV-50 exhibits a remarkable CH 4 production rate of 81.7 mmol g −1 h −1 with a 100% CH 4 selectivity under a 1.5 W cm −2 light illumination, which is significantly higher than commercial Ru/TiO 2 and other reported catalysts. We reveal that the superior photocatalytic CO 2 methanation performance is mainly due to the synergistic effect of Ru doping and TiO 2 with tunable oxygen vacancies. Impressively, the light rather than thermal effect is confirmed as the main influencing factor by experimental studies. In addition, in situ spectroscopic technology is performed to investigate the CO 2 methanation reaction pathway. This work will open an avenue to design and prepare highly efficient photocatalyst with tunable oxygen vacancies for CO 2 conversion and other related applications.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Hu Canyu,Chen Xing,Low Jingxiang,Yang Yaw-Wen,Li Hao,Wu Di,Chen Shuangming,Jin Jianbo,Li He,Ju Huanxin,Wang Chia-Hsin,Lu Zhou,Long Ran,Song Li,Xiong Yujie
Imitating the natural photosynthesis to synthesize hydrocarbon fuels represents a viable strategy for solar-to-chemical energy conversion, where utilizing low-energy photons, especially near-infrared photons, has been the ultimate yet challenging aim to further improving conversion efficiency. Plasmonic metals have proven their ability in absorbing low-energy photons, however, it remains an obstacle in effectively coupling this energy into reactant molecules. Here we report the broadband plasmon-induced CO 2 reduction reaction with water, which achieves a CH 4 production rate of 0.55 mmol g −1 h −1 with 100% selectivity to hydrocarbon products under 400 mW cm −2 full-spectrum light illumination and an apparent quantum efficiency of 0.38% at 800 nm illumination. We find that the enhanced local electric field plays an irreplaceable role in efficient multiphoton absorption and selective energy transfer for such an excellent light-driven catalytic performance. This work paves the way to the technique for low-energy photon utilization.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shihai Cao,Hao Liu,Zhenhe Jia,Meng Guo,Wentong Gao,Zhaohan Ding,Weijie Yang,Liang Chen,Wenjing Wang
CO 2 photoreduction by carbon nitride (CN) is an appealing idea, but its current efficiency remains daunting for practical viability. The amine-functionalized CN with controllable adsorption groups was prepared by carboxylation and acylation reactions. The carboxylation and amine-functionalization process preserved the crystalline structure of CN but exfoliated bulk CN to thin layers avoiding its agglomeration. With the successful graft of EDA, the amounts of –NH 2 groups for 24-CN-EDA increased remarkably compared with bulk CN. EDA-functionalization benefited CO 2 reduction activity of CN with varying amounts of amino groups. The CO yield of 24-CN-EDA was 5.92 folds to bulk CN. The enhancement was mainly triggered by the enlarged CO 2 adsorption capacity and reduced charge transfer resistance, rather than band structure and light absorption. Moreover, DFT calculations suggest that the graft of EDA on CN nanosheets possesses reduced energy barrier for CO 2 reduction into CO via enhancing CO* desorption and CO formation.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Ren Wu,Agula Bao
With the development of large-scale animal husbandry, large amounts of manure have brought great harm to the ecological environment, thus limiting sustainable development of human and animal husbandry. Biomass carbon has been extensively studied as an adsorption material. The rational use of cow dung as biomass has important research significance for the ecological environment. However, most previous work has directly converted biomass to carbon, which limits its application due to the poor quality stability of the biomass porous carbon and large variations in performance resulting from the complexity of biomass composition and microstructure. In this work, porous carbons were prepared after pretreatment of cow dung with NaOH-urea solution to extract cellulose and activate KOH. The results showed that the materials prepared under the optimal conditions (pre-carbonization temperature of 600 °C, cellulose-to-KOH ratio of 1:1) exhibited an ultrahigh specific surface area (1345 m 2 /g) and micropore ratio (74.24%). The capacities for adsorption of CO 2 at 273 K and 298 K and 1 bar were as high as 4.61 mmol/g and 3.26 mmol/g, respectively. This study expands the application range for cellulose and has significance for future preparation of porous carbon materials by extracting cellulose from biomass.
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高影响因子
ENERGY
·
2023
·
IF 9
Fa-Ping Liu,Ai-Rong Li,Cheng Wang,Yu-Ling Ma
The complex kinetic process of CO 2 hydrate formation limits its applications of CO 2 capture and sequestration et al. In this work, the effects of metal-based ionic liquids with different cations and anions on CO 2 hydrate nucleation and growth was studied. The results showed that CO 2 hydrate nucleation was promoted by the anions of [NiCl 3 ] - , [MnCl 3 ] - , [FeCl 4 ] - , [C 8 MIM] + and [C 16 MIM] + ions due to the enhancement of local hydrogen-bonding network to construct crystal nuclei. The induction time of CO 2 hydrate nucleation was decreased by 75.0% in the [C 16 MIM]FeCl 4 aqueous solution. However, CO 2 hydrate nucleation was inhibited by [C 2 MIM] + and [ZnCl 3 ] - anion. The gas storage capacity of CO 2 hydrate was increased by mass transfer channels around the metal complex anions which could accelerate the diffusion rate of H 2 O and CO 2 molecules. The co-effect between [C 16 MIM] + cations and [FeCl 4 ] - anions on CO 2 hydrate growth was the strongest, which increased gas storage capacity by 16.1%. Hence, CO 2 hydrate formation can be controlled and tuned by changing cations and anions of metal-based ionic liquids.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiaozhi Xu,Lingyu Zhang,Biao Li,Zeya Yang,Jingbin Han
Two-dimensional (2D) nanosheets with thickness of one to several atoms serve as ideal building units for separation membranes. Assembling 2D nanosheets into layered stacks with well-defined spacing as molecular separation channels is still a huge challenge. Herein, we report the construction of ultrathin membranes with layered double hydroxides (LDHs) nanosheets, polyacrylic acid (PAA) and polyethyleneimine (PEI) alternately deposited on porous substrates based on layer-by-layer assembly. The chemical tuning of PEI leads to an accurate regulation of interlayer spacing in angstrom scale, resulting in selective nanochannels for CO 2 permeation. The laminar membranes with CO 2 transport-facilitated channels exhibit excellent gas separation performance and exceed the limit of the state-of-the-art membranes with CO 2 permeance of 1068 GPU (1 GPU = 1 × 10 -6 cm 3 (STP) cm −2 s −1 cmHg −1 ), CO 2 /N 2 and CO 2 /CH 4 selectivity of 126 and 330 respectively. It is revealed the as-prepared nanofilms with strong adsorption enthalpy overcome the energy barrier of CO 2 molecules entering into and diffusing through the nanochannels. The strategy demonstrated in this work would open up new avenues for effective CO 2 separation and capture in recycling of carbon resources.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Wenqin Ling,Zhengguang Zou,Shuchao Zhang,Xiaoxiao Peng,Shiying Luo,Xin Tang,Jing Geng
Heteroatom doping has always been a common modification method for lithium-ion batteries (LIBs) cathodes. The addition of guest heteroatoms to the material can adjust the microstructure of the host material, and enlarge the lattice spacing or form the vacancy defect of oxygen, which can effectively improve the Electrochemical performance of materials. Herein, CO 2 -modified VO 2 (B) nanorods were synthesized via a simple one-step hydrothermal method . Thanks to the extended layer spacing in VO 2 (B) that results from CO 2 small molecules, the synthesized CO 2 -VO 2 electrode exhibits a high initial capacity of 251.1 mA g −1 at 100 mA g −1 , and a capacity retention of 81.8 % after 80 cycles. It is worth noting that the CO 2 -VO 2 electrode also has a high rate capacity (170.0 mAh g −1 at 1 A g −1 ), and the capacity recovery rate can reach 84.5 % even under the condition of variable current. Further studies showed that the role of CO 2 small molecules as a pillar in the interlayer of VO 2 (B) and a weak electrostatic attraction between O CO2 and Li + existed, resulting in a robust crystal structure and convenient Li-ion diffusion conditions during the (de)intercalation of lithium ions in VO 2 (B). This study opens the way for further exploration of the application of small molecule doping in the field of lithium-ion batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Dongfang Zhao,Shoulong Dong,Liju Bai,Dongyang Li,Helei Liu
The concentration profiles of all chemicals obtained in the Amine-CO 2 -H 2 O system based on the Vapor-liquid equilibrium (VLE) plots are essential for the analysis and understanding of the kinetics. This work aims at obtaining accurate and reliable VLE plots of 3DMA1P via both experimental and mathematical methods. VLE plots are essential for understanding the reaction process and mechanism of carbon dioxide absorption into amine solutions. The experiments were conducted over a concentration range of 1 ∼ 2 mol/L, temperature of 298 K, and CO 2 partial pressure of 15 kPa. Regarding the experimental method, 13 C NMR detection was performed to generate concentrations of Amine and AmineH + based on the protonation calibration equation. The results showed that the 13 C NMR method had little difference between the results of mass conservation calculation and charge conservation calculation under different CO 2 loading. Among the mathematical methods, the results obtained by the pH method involving charge conservation were quite different from those calculated by mass conservation, while the D-M model method strictly following the theoretical system satisfied both the mass and charge conservation. The distribution curves of the concentration of each species obtained by the three methods were compared. It was found that 13 C NMR and D-M model method could secure closer and more accurate results than the pH method. In conclusion, both the 13 C NMR method and the D-M model method plots are useful for obtaining accurate and reliable VLE plots for the 3DMA1P-CO 2 -H 2 O system, as well as for other monoamine and mixed amine systems.
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