CARBON
·
2019
·
IF 7.466
Yawei Yue,Yangye Sun,Can Tang,Bing Liu,Zhe Ji,Anqi Hu,Bin Shen,Zizhong Zhang,Zhengzong Sun
To reverse the ever-increasing trend of the CO 2 concentration in the atmosphere, human needs to develop a killer “catalyst”, which could convert the anthropogenic CO 2 back into high value-added or energy-storage molecules, not under the natural photosynthesis Calvin cycle, but through an artificial CO 2 reduction pathway. In the race to this emergent technology, the electrochemical reduction of CO 2 (CO 2 RR) with carbon based catalyst becomes one of the frontrunners. However, the carbon-based catalysts are genetically complex, with edge, strain, intrinsic topological defect, and doping effects, coexisting and affecting the catalysis behavior. Without a relative activity ranking system under the same metrics, unveiling the mechanism and improving the catalyst would become formidable. Here we assessed different carbon materials’ CO 2 RR performance under standard experimental conditions. The catalytic activities were evaluated and sequenced by their cathodic potential, characterized with the peak CO faradic efficiency . The doping effect is leading in the sequence, followed with the other three factors, all of which are superior to the pristine sp 2 carbon material.
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JOURNAL OF ORGANIC CHEMISTRY
·
2023
·
IF 3.6
Yunying Yan,Jianjun Hao,Fenfen Xie,Fen Han,Linhai Jing,Pan Han
Magnesium-mediated reductive carboxylation of p-QMs with CO2 via an Umpolung strategy has been developed, which can be used for the preparation of various aryl acetic acids. This protocol featured high atom economy, mild conditions, and operational simplicity. The creation of this Umpolung carboxylation of p-QMs will unprecedentedly extend the application of p-QMs to nucleophilic reagents.
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DOI
PubMed
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2016
·Vol. 32
·期 3
·605-610
·
IF 0.844
CHEN Feng-Feng,DONG Yan,SANG Xiao-Yan,ZHOU Yan,TAO Duan-Jian
Four tetrabutylphosphonium carboxylate ionic liquids ([P4444][CA]) were prepared, and their densities, viscosities, refractive indices, and conductivities were measured and correlated with thermodynamic and empirical equations in the temperature range of 298.15-348.15 K.
The influence of temperature on these four properties of [P4444][CA] was discussed, and their thermal expansion coefficient values were calculated. The CO2 absorption capacity of [P4444][CA] was studied at 313.15 K and 100 kPa. The results indicated that [P4444][Buty]
had the highest CO2 capture capacity among these ionic liquids, with an absorption capacity of 0.4 mol·mol-1 and balance time of less than 5 min.
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ACS Catalysis
·
2023
·
IF 12.9
Lei Xiong,Xianbiao Fu,Yu Zhou,Pei Nian,Zheng Wang,Qin Yue
Electrochemical CO2-to-CO conversion is a significant alternative to lower CO2 emission and build carbon-neutral processes, as well as produce CO, which can directly serve as a syngas precursor for Fischer–Tropsch synthesis. However, the easy water flooding of the gas diffusion electrode (GDE) employed in a flow cell during CO2 reduction reaction (CO2RR) electrolysis remains a tough problem. Consequently, it breaks the electrolyte/catalyst/CO2 triphase interface and lowers the FECO. Herein, the combined inarching of amino-substituted cobalt phthalocyanine (CoPc-NH2) and octadecylamine (ODA) onto the surface of the CNT via an amide bond was designed and fabricated. The obtained composite catalyst, labeled as CoPc-CNT-ODA, shows atomically dispersed metal active sites endowed with superior and stable hydrophobicity. When applied to CO2RR in a flow cell, the CoPc-CNT-ODA electrode displays a high CO faradic efficiency (FECO) of 97.7% and a partial current density (jCO) of 154.8 mA·cm–2 at an applied potential of −1.0 V (vs RHE). Moreover, the FECO values are all above 90% from −0.8 to −1.2 V (vs RHE). Even after electrolyzing at −1.0 V for 12 h, the FECO still remains at 88.3%, implying the superior stability of the CoPc-CNT-ODA electrode. The proposed methodology for GDE/catalyst improvement can be extended to other triphase interfaces involved in catalytic systems.
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JOURNAL OF CHEMICAL ENGINEERING OF JAPAN
·
2015
·Vol. 48
·期 4
·268-275
·
IF 0.644
Da-Niu Cai,Kuan Huang,Xiao-Min Zhang,Xing-Bang Hu,You-Ting Wu
Amino acids were used to modify macroreticular ion exchange resin for the adsorptive capture of CO2. Adsorption isotherms, adsorption rate curves, heats of adsorption, and gas separation performance were determined. It is found that the adsorption capacity of the resin increases significantly after the loading of amino acids. The adsorption progresses rapidly and reaches equilibrium within 3 min. The adsorption capacity decreases with the increasing temperature, and room temperature is a suitable condition that enables high adsorption of CO2. The adsorbent can be promoted by water vapor in removing CO2 effectively from gas mixtures. Ten continuous adsorption–desorption cycles was performed, showing that the adsorbent is of good regeneration performance and the adsorption capacity keeps at about 0.9 mmol/g after regeneration.
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DOI
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Science China-Chemistry
·
2019
·Vol. 62
·期 12
·1710-1719
·
IF 6.085
Wang Guishuo,Luo Ran,Yang Chengsheng,Song Jimin,Xiong Chuanye,Tian Hao,Zhao Zhi-Jian,Mu Rentao,Gong Jinlong
Metal oxide-promoted Rh-based catalysts have been widely used for CO 2 hydrogenation, especially for the ethanol synthesis. However, this reaction usually suffers low CO 2 conversion and alcohols selectivity due to the formation of byproducts methane and CO. This paper describes an efficient vanadium oxide promoted Rh-based catalysts confined in mesopore MCM-41. The Rh-0.3VO x /MCM-41 catalyst shows superior conversion (~12%) and ethanol selectivity (~24%) for CO 2 hydrogenation. The promoting effect can be attributed to the synergism of high Rh dispersion by the confinement effect of MCM-41 and the formation of VO x -Rh interface sites. Experimental and theoretical results indicate the formation of til-CO at VO x -Rh interface sites is easily dissociated into *CH x , and then *CH x can be inserted by CO to form CH 3 CO*, followed by CH 3 CO* hydrogenation to ethanol.
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DOI
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Haiyang Zhang,Ruili Guo,Jinli Zhang,Xueqin Li
Mixed matrix membranes (MMMs) have exhibited advantages in overcoming the trade-off effect, although it is still intensively demanded in the design of multifunctional fillers to improve CO2 separation performance. At present, MMMs with transport channels present an effective strategy to obtain ultrahigh CO2 permselectivity. In this work, Pebax-based MMMs was fabricated by incorporating nanocapsules (NCs), whose exterior, interior and transverse shell surfaces contained abundant carboxylic acid groups. NCs, similar to vesicles in cells, provide favorable physical and chemical microenvironments to the constructed CO2 transport channels, enhancing the CO2 permselectivity via both a facilitated transport mechanism and a solution-diffusion mechanism. CO2 permselectivity of MMMs doped with 20 wt % NCs surpassed the 2008 Robeson limit; an increase in CO2 permeability was up to 1431 ± 35 Barrer for pure gas, which was a 362% enhancement from the pure membrane, and an increase of the CO2/CH4 and CO2/N2 ideal selectivities to 46 ± 1.4 and 69 ± 2.7, corresponding to 44% and 23% enhancements from the pure membrane, respectively. This study provides an ingenious strategy to enhance the gas permselectivity of MMMs.
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DOI
PubMed
高影响因子
LETTERS IN ORGANIC CHEMISTRY
·
2023
·Vol. 20
·期 4
·370-375
·
IF 0.8
Chai Mengliang,Wu Fengtian,Wu Ling
The process of hydrogen bond donor accelerating the cycloaddition of epoxides with CO2 is green access to high economic value cyclocarbonate derivatives. However, hydrogen bond donor still has certain limitations such as poor biocompatibility and narrow substrate
scope. Our group found that folic acid could promote the coupling reaction of epoxides and CO2 through hydrogen-bonding. The reaction was used to synthesize various cyclocarbonate derivatives in good to high yields with the aid of folic acid and TBAB. In addition, benzoic
acids and 2,4-quinazoline dione were synthesized in the presence of CuCl2/folic acid and PdCl2/folic acid, respectively. The reaction mechanism was proposed based on previous reports and control experiments.
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NANO
·
2019
·
IF 1.293
Hongning Wang,Chao Xu,Yongsheng Zhou,Wenpu Zhao,Jing Zhong,Weiqiu Huang,Ruoyu Chen
Hierarchical N-doped carbon nanotubes (NCTs) with controllable aspect ratios were developed for CO 2 adsorption. In this work, NCTs were synthesized by coating different amounts of 3-aminophenol/formaldehyde resin (APF) on the outer layer of silica nanotubes, carbonizing in N 2 at 700 ∘ C and removing the silica and Ni template by hydrofluoric acid etching. The obtained NCTs were activated by K 2 CO 3 . After activation, micropores on the activated N-doped carbon nanotubes (ANCTs) were enriched, the micro-surface area and pore volume of ANCT-1.0 reached 1195 m 2 g − 1 and 0.45 cm 3 g − 1 , respectively, and the corresponding adsorption capacity increased by 50% (4.50 mmol g − 1 at 0 ∘ C and 1 bar). Moreover, ANCT-1.0 maintained a high stability throughout consecutive adsorption–desorption cycles. The advantages of hierarchical N-doped carbon nanotubes, including their meso–microporous structures, high geometric aspect ratio and good stability, make them valuable and promising materials to capture carbon dioxide.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Qinghua Qu,Yuqiao Jiang,Linyan Cheng,Qingyuan Xue,Ranran Li,Cheng Fang,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan
Covalent organic frameworks (COFs) with high specific surface area, ordered pore wall, modified porous surface and customizable chemical structure have been widely used in CO 2 capture. However, the screening of functionalized COFs suitable for CO 2 capture still relies on experiments, which will require a long experimental period with blindness and randomness. Herein, we chosed three electron withdrawing groups (–NO 2 , –CN and −Br) and three electron donating groups (–CH 2 NH 2 , –CH 3 , –OCH 3 ) to explore the effect of electron withdrawing ability of functional groups on the CO 2 adsorption capacity. Grand canonical Monte Carlo (GCMC) method was used to simulate the adsorption capacity of CO 2 over X-TpBD-COFs (X=–NO 2 , –CN, −Br, –CH 2 NH 2 , –CH 3 , –OCH 3 ). As the result, NO 2 -TpBD-COF had the highest adsorption capacity among the six functionalized X-TpBD-COFs at 100 kPa and 25 ℃ (49.37 cm 3 /g), while OCH 3 -TpBD-COF had the lowest adsorption capacity among them (23.51 cm 3 /g at 25 ℃ and 100 kPa). The order of binding energy was basically the same as the order of adsorption capacity when the synergistic interactions between functional groups and oxygen atoms in Tp were considered according to density functional theory (DFT). Molecular dynamics (MD) showed that the diffusion and distribution of CO 2 were mainly effected by pore structures. To verify the simulation results, NO 2 -TpBD-COF and OCH 3 -TpBD-COF were successfully prepared by solvothermal method. The CO 2 adsorption capacities of these two COFs were basically consistent with the conclusion obtained by the simulations. This study provided a way for simulation to guide accurate and rapid experimental design of COF materials for CO 2 capture.
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产品关联
DOI
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iScience
·
2024
·
IF 4.6
Jielin Huang,Jie Wang,Haonan Duan,Li Dong,Songsong Chen,Junping Zhang,Xiangping Zhang
Acidic and basic sites of catalysts are essential for CO 2 capture and activation. In this work, Zr, N-ZnO/ZnAl-LDH-IL composites in ionic liquid and methanol systems were fabricated, and applied to catalyze the synthesis of ethylene carbonate (EC) from ethylene glycol (EG) and CO 2 with about 4.76 mmol EC g Cat. −1 h −1 . The composites showed more strong basic sites due to the effective induction of reactive groups on the catalyst surface by Zr doping, resulting in an increase of pyridinic-N groups from 5.48% to 22.25%. More C atoms adjacent to pyridinic-N as strong basic sites was conducive to the activation of CO 2 and EG. In addition, the possible catalytic pathway and mechanism of the composites for synthesizing EC as well as the doping of La, Fe, Ce, and Cu were also investigated, which provides an effective strategy for regulating the acid-base centers on the catalyst surface through ionic liquids and methanol solvents.
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Sheng Chang,Yimin Xuan,Jingjing Duan,Kai Zhang
Electrochemical CO 2 conversion into valuable products provides a promising solution for achieving a carbon-neutral energy cycle. Herein, an active and stable Bi/Nafion interface is fabricated over Bi nanosheets with the modification of Nafion, which exhibits superior CO 2 conversion with formate selectivity of above 95% in a wide potential range, partial current density of 72.12 mA cm −2 at − 1.07 V vs. RHE in H-type cell. The extraordinary CO 2 reduction performance could be ascribed to a high CO 2 permeability and enhanced local proton activity at the Bi/Nafion interface, which leads to promoted CO 2 adsorption and feasible proton-coupled electron transfer during the CO 2 reduction process. Computational investigations reveal the modification of Nafion offers a comfortable platform to enable the key intermediate *OCHO to be stable. This work offers a valuable insight into interfacial manipulation of electrodes to convert CO 2 to valuable products.
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