CHEMICAL ENGINEERING SCIENCE
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2018
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IF 3.306
Xunan Hou,Linzhou Zhuang,Beibei Ma,Shuixia Chen,Hui He,Fengqin Yin
In this work, we report a new route to improve the CO 2 adsorption performance of solid amine adsorbents. Platelet mesoporous silicas with abundant surface silanols were prepared by emulsion synthesis followed by simple solvent extraction. These silanol-rich silica particles were then functionalized with branched polyethyleneimine (BPEI) by grafting or impregnation to prepare CO 2 adsorbents. Silanol-rich silicas grafted with BPEI exhibited 70% higher amine density and 47% higher CO 2 adsorption capacity than its calcined counterpart. The adsorbent achieved a maximum CO 2 adsorption efficiency up to 13.82 mmol CO 2 /g-BPEI. Adsorbed species found in the infrared spectra suggested that silanols may contribute to the enhanced CO 2 adsorption efficiency on grafted amines. Silanol-rich silica functionalized with BPEI retained more porosity than its calcined counterparts, which may account for its superior CO 2 adsorption capacity. Silanol-rich silica impregnated with amines achieved the highest CO 2 adsorption efficiency ever reported (5.65 mmol/g, 526.7 mg/g-BPEI). Adsorption kinetic modeling confirmed that silanol-rich adsorbent provides better CO 2 diffusion pathways. These potential benefits of silanol-amine interaction, coupled with platelet mesoporous structure and branched polyamine chains, opens a new pathway to high-performance adsorbents for CO 2 capture.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
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IF 4.229
Aisheng Huang,Bo Feng
Pristine graphene oxide (GO) sheets were pretreated with polyethyleneimine (PEI) to prepare PEI-modified GO (PEI-GO), which was further inserted with ZIF-8 crystals to form a novel PEI-GO@ZIF-8 nanocomposite for CO 2 capture. The good dispersion of PEI and interlayer growth of ZIF-8 within the GO sheets is helpful for high CO 2 adsorption. Therefore, the PEI-GO@ZIF-8 nanocomposite show high surface area and enhanced CO 2 adsorption capacity . The adsorption capacity of the PEI-GO@ZIF-8 nanocomposite was six times higher than that of the pristine GO and ZIF-8. The CO 2 /N 2 adsorption selectivity was significantly improved due to amine groups loading which provide more sites for CO 2 adsorption. The preferential adsorption of CO 2 over N 2 makes PEI-GO@ZIF-8 nanocomposite be a promising candidate in the field of CO 2 capture.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2018
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IF 3.649
Mingqiang Liu,Lishu Shao,Jianhan Huang,You-Nian Liu
The O-containing hyper-cross-linked polymers were synthesized from phenol (2-naphthol) and formaldehyde dimethyl acetal by a simple one-step Friedel-Crafts reaction, they were subsequently carbonized using KOH as the activating agent, and their adsorption to CO 2 was carefully tested. The results indicated that these samples had a high Brunauer-Emmett-Teller surface area (up to 2241 m 2 /g), pore volume (up to 1.20 cm 3 /g), CO 2 uptake (up to 6.3 mmol/g at 273 K and 1.0 bar), and CO 2 /N 2 selectivity (up to 96 for the HCPs, and 22.5 for the porous carbon). In particular, the CO 2 adsorption was highly dependent on the ultramicropore volume (pore width<0.7 nm), while the CO 2 /N 2 selectivity mainly relied on the oxygen content and the ultramicropore structure.
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International Journal of Electrochemical Science
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2024
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IF 1.3
Wenhui Dong,Xinyuan Sun,Qianqian Niu,Yun Zhu,Baokang Jin
Phenylacetic acid derivatives, including 1-naphthaleneacetic acid, hold crucial applications in various domains. Traditional synthesis methods often involve intricate steps or the use of expensive and polluting heavy metal catalysts. This paper presents an electrochemical approach for efficiently producing valuable compounds like 1-naphthaleneacetic acid and other phenylacetic acid analogs through the reduction of benzyl halides, such as 1-chloromethyl naphthalene, in the presence of CO 2 . At the same time as preparing phenylacetic acid, the resource utilization of CO 2 is realized. Six kinds of carboxy analogs were synthesized by potentiostatic electrolysis of benzyl halides in acetonitrile with CO 2 as a co-reactant and tetraethyl ammonium tetrafluoroborate as an electrolyte. The electrochemical reduction products were confirmed structurally through NMR, mass spectrometry, and other techniques. The Faraday electrolysis efficiencies ranged from 82 % to 94 %, with 72.5–92.9 % conversions. The study delves into the electron transfer mechanism using cyclic voltammetry and in situ FT-IR spectroelectrochemistry. The reduction process on silver electrodes under a CO 2 atmosphere was identified as an irreversible two-electron process, generating a monovalent anion that attacks CO 2 to yield the respective carboxyl analogs.
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Journal of Energy Chemistry
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2024
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IF 14
Haocheng Xiong,Donghuan Wu,Haonan Li,Andrew Li,Qikun Hu,Siyao Song,Bingjun Xu,Qi Lu
Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO 2 emissions, as bicarbonate can be efficiently generated from the capture of atmospheric CO 2 using alkaline solutions with reactive absorption. In this work, we present a CO 2 -mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm 2 electrode area. Our electrolysis achieved selectivities exceeding 75% for formate at a total current of 2.5 A, achieving formate concentrations up to 1.2 M and yields as high as 95% over extended periods. The techno-economic assessment confirmed the economic viability of the process, highlighting the potential for bicarbonate electrolysis as a sustainable method for producing valuable chemicals.
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NANOTECHNOLOGY
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2024
·Vol. 35
·期 19
·195605
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IF 2.9
Shuo Wang,Haotian Yin,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic reduction of carbon dioxide is a technology that effectively utilizes CO2 and solar energy. Sodium niobate (NaNbO3) has received much attention in the field of photocatalysis due to its excellent photocatalytic properties. However, the application of NaNbO3 in the field of photocatalysis is still limited by poor reaction to visible light and easy recombination of photo-generated carriers. Heterojunction with g-C3N4 to construct core–shell structure can effectively improve the above problems. Combining the two can design a core–shell composite material that is beneficial for photocatalytic reduction of CO2. Herein, we prepared a core–shell heterojunction g-C3N4/NaNbO3 by uniformly impregnating urea on the surface of NaNbO3 chromium nanofibers with NaNbO3 nanofibers prepared by electrospinning as a catalyst carrier, and urea as a precursor of g-C3N4. The core–shell structure of g-C3N4/NaNbO3 was verified by a series of characterization methods such as XPS, XRD, and TEM. It was found that under the same conditions, the methanol yield of core–shell g-C3N4/NaNbO3 was 12.86 μmol·g−1·h−1, which is twice that of pure NaNbO3 (6.67 μmol·g−1·h−1). This article highlights an impregnation method to build core–shell structures for improved photocatalytic reduction of CO2.
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LANGMUIR
·
2024
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IF 3.7
Xinzi Wu,Jiawei Ruan,Lifang Chen,Zhiwen Qi
The development of aqueous absorbents for CO2 capture is significantly important to reduce global industrial gas emissions through high regeneration efficiency and low energy consumption. Herein, we newly designed and prepared a dihydroxylated ionic liquid (IL) bis(2-hydroxyethyl)dimethylammonium 1,2,4-triazole ([N1,1,2OH,2OH][TZ]) for highly efficient CO2 absorption through anion–cation cooperative interactions. A superior capacity of 1.33 mol of CO2 per mol of IL and excellent reversibility have been achieved by the introduction of dihydroxy sites on the ammonium-based Tz IL. 1H and 13C nuclear magnetic resonance, Fourier transform infrared, and quantum chemical calculations demonstrate bihydroxyl-cooperative absorption of CO2 via hydrogen bond interaction between the cation and anion of the IL. The theory calculation shows that IL displays a superlow reactive absorption enthalpy, favorable to the reversible CO2 absorption, which can maintain an initial absorption capacity of 98.5% with the cycle numbers of 100, implying the facile regeneration and superlow energy consumption. Thus, the functionalized ILs toward group cooperative gas absorption and excellent reversibility may open a door to designing new materials for enhancing CO2 absorption and utilization.
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ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Lulu Zhao,Huilin Hou,Shuo Wang,Lin Wang,Yang Yang,Chris R. Bowen,Jinguo Wang,Ziyi Liao,Dongjiang Yang,Ruifang Yan,Weiyou Yang
Despite the development of a range of photocatalysts for CO 2 reduction, the practical applications are significantly limited by low conversion efficiencies and their reliance on sacrificial agents, which are rooted in thermodynamic and kinetic challenges related to CO 2 conversion. Here, the engineering of Co single atoms in ultrathin single-crystal BiOCl nanosheets for boosted photocatalytic CO 2 reduction is reported. The engineering of Co atoms modulates the distribution of photogenerated charges at the catalyst surface, controlling key surface reaction dynamics and suppressing surface electron-hole recombination. This modulation also improves light absorption and enhances CO 2 adsorption and activation, leading to more efficient surface reactions. Notably, CO 2 is stably adsorbed onto the (001) face of BiOCl through a Bi-O-C(= O)-Co-O coordination unit, which lowers the activation energy for CO 2 reduction and reduces the formation energy of COOH − intermediates. As a result, the BiOCl photocatalysts achieve a CO formation rate of 183.9 µmol g −1 h −1 , when irradiated with a 300 W Xe lamp without cocatalysts or sacrificial agents. It represents an ≈13-fold increase compared to that of pristine BiOCl, and surpasses most reported Bi-based photocatalysts to date. Current work provides valuable insights into engineering of single atoms for developing advanced CO 2 -reduction photocatalysts.
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AICHE JOURNAL
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2024
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IF 3.5
Dongyu Jin,Wenyu Ge,Zhiyong Zhou,Yuming Tu,Chenchan Du,Zhongqi Ren
Porous liquids (PLs) with unique porous frameworks and good flow properties can achieve coupling enhancement for CO 2 capture and conversion. In this paper, a series of novel PLs were designed and synthesized using UiO-66 as the framework and novel bi-cationic ionic liquids (ILs) as an excluded solvent. The prepared PLs showed significant improvement in CO 2 uptake capacity over ILs at different pressures and exhibited excellent CO 2 catalytic conversion performance, exceeding the sum of the effects of ILs and UiO-66. Especially at low pressure, the PLs still showed excellent catalytic performance, but the catalytic performance of the corresponding ILs was significantly reduced, which was due to the rapid adsorption and conversion of CO 2 by the porous framework of UiO-66 to improve the CO 2 uptake and transfer efficiency within the ILs, thus achieving coupling enhancement. It can provide a new way to realize the efficient conversion of CO 2 under milder conditions.
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Science Advances
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2024
·Vol. 10
·期 47
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IF 11.7
Rongrong Pan,Qi Wang,Yan Zhao,Zhendong Feng,Yanjun Xu,Zhuan Wang,Yapeng Li,Xiuming Zhang,Haoqing Zhang,Jia Liu,Xiang-Kui Gu,Jiangwei Zhang,Yuxiang Weng,Jiatao Zhang
Sluggish surface reaction is a critical factor that strongly governs the efficiency of photocatalytic solar fuel production, particularly in CO2-to-ethanol photoconversion. Here, inspired by the principles underlying enzyme catalytic proficiency and specificity, we report a biomimetic photocatalyst that affords superior CO2-to-ethanol photoreduction efficiency (5.5 millimoles gram−1 hour−1 in average with 98.2% selectivity) distinctly surpassing the state of the art. The key is to create a class of catalytic pocket, which contains spatially organized NH2…Cu-Se(-Zn) multiple functionalities at close range, over ZnSe colloidal quantum wells. Such structure offers a platform to mimic the concerted cooperation between the active site and surrounding secondary/outer coordination spheres in enzyme catalysis. This is manifested by the chemical adsorption and activation of CO2 via a bent geometry, favorable stabilization toward a variety of important intermediates, promotion of multielectron/proton transfer processes, etc. These results highlight the potential of incorporating enzyme-like features into the design of photocatalysts to overcome the challenges in CO2 reduction.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Ting He,Shuang Yao,Dejian Chen,Zhaoyun Sun,Xiaoyun Wang,Keyi Wang,Jiangwei Chen,Qingguo Li,Rizhi Chen,Yawei Wang,Zhaoliang Cui
Membrane oxygenator performs lung function in the Extra-corporeal Membrane Oxygenation (ECMO) system. In the clinical use, to ensure the balance of gas exchange of patient’s body, the gas-blood exchange membrane is required to possess CO 2 /O 2 selectivity, which is suggested to be in the range of 10-12. In our work, the molecular dynamics simulation results displayed that the amino-functionalized Zr-MOFs provides fast transport channels for CO 2 molecules because of the enhancement of the adsorption and diffusion ability for CO 2 . Therefore, we chose organic ligands with abundant CO 2 -philic groups to synthesize target amino-functionalized Zr-MOFs, and then dispersed them into medical-grade PDMS solution to study the separation performance of CO 2 /O 2 . On the basis of constructing anti-leakage coating layer, biomimetic gas channels were designed to increase the clearance rate of CO 2 . Experimental results exhibited that the CO 2 /O 2 selectivity of (NH 2 ) 2 -UiO-66/PDMS MMM was as high as 11.19, which was basically consistent with the simulation results. The obtained amino-functionalized Zr-MOF/PDMS coating layer displayed favorable biocompatibility and biosafety. Meanwhile, the construction of biomimetic channel solves the difficult problem of CO 2 removal in PMP membrane, which verifies the feasibility of applying porous materials to gas-blood exchange membranes in the ECMO system.
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Progress in Natural Science-Materials International
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2024
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IF 4.8
Shijia Liu,Haibin Wang,Xi Wang,Jieshu Zhou,Hongyan Liang
Electroreduction of CO 2 for formic acid production has been regarded as an efficient option for CO 2 utilization. However, under high current, achieving high selectivity for formic acid is challenging, which cannot meet industrial demands. Herein, we reported a type of Bi/In(OH) 3 (BIO) heterojunction reconstructed from Bi 2 S 3 /In(OH) 3 during electrochemical process, in which In(OH) 3 was applied to modulate the electronic structure of Bi. This strategy efficiently enhanced the ∗OCHO intermediates adsorption and lead to a decent selectivity towards formic acid under high current density. BIO displays faraday efficiency of formic acid beyond 95 % across a wide range current density of 200–400 mA cm −2 , where the highest value reached 97.7 % at 400 mA cm −2 . This work clarified the mechanism of CO 2 electroreduction to HCOOH on heterojunction, guiding the design of advanced catalysts.
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