Journal of Materials Chemistry A
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2023
·Vol. 11
·期 8
·4261-4271
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IF 11.9
Yuxin Xie,Chenghao Yao,Lei Li,Zhan Lin
The light-triggered CO2 catalytic reduction process of high efficiency is highly desirable but challenging. Herein, we present two viologen-based metal–organic frameworks (M-VOF, where M = Co and Ni) as ideal platforms for photocatalytic CO2 reduction. Co-VOF exhibits a high CO evolution rate of 458.66 μmol g−1 h−1 under light irradiation, while Ni-VOF provides a CO evolution rate of 52.33 μmol g−1 h−1 with superior durability. Experimental studies reveal that the viologen-based frameworks play an important role in the transfer and separation of the charge carriers in the catalytic system. This work provides not only a superior Co-VOF catalyst but also promotes in-depth insight into the structure–activity relationships toward the activation and photoreduction of CO2.
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CHEMICAL ENGINEERING JOURNAL
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2022
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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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APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Dehao Kong,Weirong Zhou,Jiayin Han,Yubing Gao,Yuan Gao,Liupeng Zhao,Peng Sun,Geyu Lu
Crystal facet engineering strategy is an effective way to regulate the exposed facets, which affect the ability of the surface to adsorb and react with gas molecules, ultimately enhancing the gas-sensing properties. In this work, Co 3 O 4 mesoporous nanosheets with dominant exposed {1 1 1} facets (Co 3 O 4 -60) or {1 1 2} facets (Co 3 O 4 -100) were synthesized by simply adjusting the condensation-reflux temperature. The sensing results toward toluene show that Co 3 O 4 -60 exhibited superior performance. According to the crystal structure analysis and work function calculations, the (1 1 1) facet composed of Co 2+ would adsorb more oxygen molecules, which have been proved by experimental characterization, facilitating the sensing efficiency. The results of X-ray photoelectron spectroscopy indicated that Co 3 O 4 -60 possesses a higher Co 2+ content and chemisorbed oxygen ratio (52.9%). Furthermore, Co 3 O 4 -60 has a high electrical conductivity and a minor apparent activation energy for toluene (38.75 kJ/mol). The gas sensor based on Co 3 O 4 -60 exhibited a response of 20.6 for 100 ppm toluene with rapid recovery and a detection limit of 1 ppm. Besides, other properties such as selectivity, repeatability, and humidity resistance were evaluated. This work evidences that crystal facet engineering is a practical approach to improving the gas-sensing properties of pure-phase Co 3 O 4 .
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2023
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IF 7.8
Hongwei Ren,Yize Liu,Ruoyao Zhang,Tengda Zhao,Jing Han,Zhiyang Zheng,Erhong Duan
The sustainable development of carbon dioxide (CO 2 ) resource requires the realization of green and efficient capture for the fossil fuel CO 2 . However, the high operation costs and biological toxicity have hampered the application. Natural deep eutectic solvents (NADESs) are efficient and green CO 2 absorbent. In this manuscript, kinds of amino acid-based NADESs were prepared successfully to improve the absorption efficiency of CO 2 capture solvent. The chemical structure of NADESs was characterized, and the thermal stability was also measured. The CO 2 capture behavior of amino acid-based NADESs was investigated. With multi-reactive sites, unstable stage and more accessibility of alkyl structure on HBA (alkyl amino acids and aromatic amino acids, especial L -Ary), and less electronegativity on HBD (EG), L -Arg/EG NADESs had lower solvation effect ( β value, 1.286) and reduced viscosity (48.33 mpa.s at 60 ºC). It behaved better absorption capacity . The optimized conditions by single-factor analysis and Response surface methodology were L -Arg/EG at the mole ratio of 1:5, 30 °C and 200 mL/min, and the absorption could reach 0.81 molCO 2 /kgNADESs. Additionally, an insight into the reaction mechanism was investigated. It was found that hydrogen-bond structure played an important role in CO 2 capture. The broken of H-O···H-N formed by amino acids and ethylene glycol promoted the formation of new bonds of -(O=)C···NHR between L -Arg/EG and CO 2 , thus achieved higher CO 2 capture. The investigated proved that the green solvent amino acid-based NADESs could be efficient absorbents for CO 2 capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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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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JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Feihan Yu,Wenxuan Wang,Yudong Li,Minshu Du,Feng Liu,Daxin Liang
TiO 2 is one of the most ideal photocatalytic materials, but its application is limited by many problems (e.g., wide band gap, easy carrier recombination). Co-catalyst with changes in valence could efficiently overcome the disadvantages above. Herein, a Fe species (Fe, Fe 2 O 3 )/TiO 2 was designed to fully utilize photogenerated charges and holes. The degradation rate of ciprofloxacin can reach 99.97%. In addition, its methane generation from photoreduction of CO 2 is 12.9 times than that of pure TiO 2 . These results are attributed to the well-designed catalyst including the combination of TiO 2 and FeO x as photocatalysts and oxygen buffers, and the dispersion of single-atom Fe clusters as cocatalysts and electron trap sites. The effect mechanism of Fe species on TiO 2 was verified by PBE DFT calculation. Finally, following a concept of thermodynamic-kinetic synergy, a new design strategy for photocatalysts is accordingly proposed, as such, the prepared catalyst is expected to be applied in the environmental remediation.
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ENERGY
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2023
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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
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2023
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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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Materials Research Express
·
2022
·Vol. 9
·期 1
·015504
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IF 2.025
Xiangwei Liu,Qian Ao,Shengyou Shi,Shuie Li
The existing CO2 absorption by deep eutectic solvents is limited by the unavoidable water absorption problem during use. In this study, we prepared three deep eutectic solvents with different alcohol aminations and added different water contents to discuss the effect of water content on the absorption of carbon dioxide by deep eutectic solvents. All deep eutectic solvents have a low melting point at room temperature as a liquid and have high thermal stability, where the choline chloride-diethanolamine deep eutectic solvents have a high viscosity. Anhydrous choline chloride-monoethanolamine deep eutectic solvents have the largest CO2 absorption, reaching 0.2715 g g−1, and the absorption of CO2 by anhydrous choline chloride-N-methyldiethanolamine deep eutectic solvents is only 0.0611 g g−1. Water content inhibited the absorption of CO2 in primary amine and secondary amine systems, whereas it enhanced the absorption of CO2 in tertiary amine systems, which was related to the reaction process of deep eutectic solvent and CO2.
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Carbon Letters
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2022
·Vol. 32
·期 3
·807-814
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IF 3.117
Ning Hui,Guo Zhihao,Wang Wenhang,Wang Xiaoshan,Yang Zhongxue,Ma Zhengguang,Tian Yangming,Wu Chenghao,Hao Jian,Wu Mingbo
Electrochemical reduction of carbon dioxide to valuable chemicals is a promising way of storing renewable energy through electric-to-chemical energy conversion, while its large-scale application is in urgent need of cheap and high-performance catalysts. Herein, we invent a convenient method to synthesize N-doped porous carbon by ammonia etching the pyrolysis carbon of petroleum pitch. We found the ammonia etching treatment not only increase the pyridinic-N content, but also enlarge the specific surface area of the petroleum pitch-based porous carbon. As a cheap and easily available catalyst for carbon dioxide electroreduction, up to 82% of Faradaic efficiency towards carbon monoxide was obtained at − 0.9 V vs the reversible hydrogen electrode in 0.1 M KHCO 3 . After a long time electrocatalysis of more than 20 h, the Faradaic efficiency of carbon monoxide remains 80%, indicating the porous carbon as made have an ultra-high stability as catalyst for carbon dioxide reduction. Our work provides a new technology to economically prepare efficient electrocatalysts for carbon dioxide reduction.
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ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200090
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IF 9.14
Wenwen Bao,Senhe Huang,Diana Tranca,Boxu Feng,Feng Qiu,Fermín Rodríguez-Hernández,Changchun Ke,Sheng Han,Xiaodong Zhuang
Graphical Beauty in balanced asymmetry : An asymmetric Co II porphyrin ( as -PorCo) is constructed with a substituent of 2,6-dimethylbenzene to enhance the charge transfer capability from carbon nanotubes to as -PorCo, resulting in large partial current density of 8 mA cm −2 and high turnover frequency of 5656 h −1 at −0.7 V vs. reversible hydrogen electrode in aqueous solution. The present study provides the new insight into molecular design of catalysts for efficient electrochemical CO 2 reduction. The electrochemical reduction of carbon dioxide (CO 2 ) based on molecular catalysts has attracted more attention, owing to their well-defined active sites and rational structural design. Metal porphyrins (PorMs) have the extended π-conjugated backbone with different transition metals, endowing them with unique CO 2 reduction properties. However, few works focus on the investigation of symmetric architecture of PorMs as well as their aggregation behavior to CO 2 reduction. In this work, a series of Co II porphyrins (PorCos) with symmetric and asymmetric substituents were used as model of molecular catalysts for CO 2 reduction. Owing to the electron donating effect of 2,6-dimethylbenzene (DMB), bandgaps of the complexes became narrower with the increasing number of DMB. As electrocatalysts, all PorCos exhibited promising electrocatalytic CO 2 reduction performance. Among the three molecules, asymmetric Co II porphyrin ( as -PorCo) showed the lowest onset potential of −288 mV and faradaic efficiencies exceeding 93 % at −0.6 V vs. reversible hydrogen electrode, which is highly competitive among the reported state-of-art porphyrin-based electrocatalysts. The CO 2 reduction performance depended on π-π stacking between PorCo with carbon nanotubes (CNTs) and adjacent PorCos, which could be readily controlled by atomically positioned DMB in PorCo. Density functional theory calculations also suggested that the charge density between PorCo and CNT was highest due to the weak steric hindrance in as -PorCo, providing the new insight into molecular design of catalysts for efficient electrochemical CO 2 reduction.
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wei Guo,Huanhao Chen
Nonthermal plasma (NTP)-assisted CO2 methanation can activate and convert stable CO2 molecules under ambient conditions as compared to conventional thermal catalysis (normal operation temperature up to 450 °C), which is a good technique to reduce CO2 emissions and simultaneously utilize the renewable energies like solar and wind. It is critical to develop a robust catalyst with good catalytic performance in order to make NTP catalytic CO2 methanation more competitive. Herein, we present a simple yet efficient synthesis of CeO2-supported Ni catalysts with yttrium (Y) as the promoter (i.e., Ni–Y/CeO2) via mechanochemical synthesis for efficient NTP catalytic CO2 methanation. The developed 7.5Ni–1Y/CeO2 catalyst demonstrated the highest energy efficiency values for CO2 conversion and CH4 yield, i.e., ∼57 gCO2 kWh–1 and ∼17 gCH4 kWh–1, respectively. The CO2-TPD and HRTEM results confirmed that the doped Y positively enhanced the basicity of the catalysts and also decreased the particle size of Ni nanoparticles, thus promoting the NTP catalytic activity of CO2 methanation. The catalyst displayed excellent short-term stability for plasma catalytic CO2 methanation over a 12 h on-stream evaluation, showing a CO2 conversion of 84.2 ± 1.8% and a CH4 selectivity of 83.3 ± 1.9%.
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