SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zongze Lv,Junqiang Han,Tao Deng,Chang Gao,Jianan Li,Changlei Qin
Integrated CO 2 capture and utilization (ICCU) is an emerging technology to reduce CO 2 emissions by greatly simplifying the processes of conventional CO 2 capture and utilization. In particular, ICCU-methanation could directly convert the low-concentration CO 2 into CH 4 using hydrogen from new energy electricity, representing an efficient Power-to-Gas route. CO 2 adsorption/catalytic materials play a crucial role for the operation of ICCU-methanation, and it is more feasible to scale up material production and avoid components interference by directly combining the sorbent and catalyst. However, it is necessary to reveal the effect of different arrangements of sorbent and catalyst on reaction characteristics of ICCU-methanation. In the work, the matching of K 2 CO 3 -doped Li 4 SiO 4 sorbent with various supported Ni-based catalyst was tested and four arrangements of sorbent and catalyst particles in a fixed-bed were investigated to understand the influences on ICCU-methanation. Results show that the presence of catalyst accelerates CO 2 supply by sorbent and achieves quicker methanation, and the promotion effect becomes more obvious with a closer contact between the sorbent and catalyst. Under optimized conditions, ICCU-methanation of uniformly mixed K-Li 4 SiO 4 and Ni/Al 2 O 3 shows an excellent performance with very stable CO 2 conversion of 95.58% and CH 4 selectivity of 93.29% during cyclic reactions.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Xinyue Hong,Youting Fang,Duobin Chao
Development of photocatalysts with both high CO 2 adsorption capacity and robust CO 2 reduction performance is promising toward carbon capture and utilization (CCU). Herein, a porous organic polymer (POP) based on molecular monomers 1,2,3,5–Tetrakis(carbazol–9–yl)–4,6–dicyanobenzene (4CzIPN) and 9–(4–([2,2′:6′,2′'–terpyridin]–4′–yl)phenyl)–9H–carbazole (CzTPY) has been prepared for metal–free photocatalytic reduction of CO 2 to CO with 94.7% selectivity in 100% aqueous medium. The POP displays a yield of CO up to 265.7 mmol g –1 , which is among the highest yields for POPs–based photocatalytic systems. More importantly, the POP also shows a high CO 2 uptake of 109.1 cm 3 g –1 (21.4 wt%) at 273 K and 1 atm. External photosensitizers or catalysts are not required in this photocatalytic system. Mechanistic studies indicate the introduction of CzTPY improved the electron transfer and charge separation. These results show a feasible way to construct POP–based photocatalysts not only capturing CO 2 efficiently but also catalyzing CO 2 reduction with a high yield by rational regulation of molecular monomers.
研究领域:
化学
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材料科学
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环境科学
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能源科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Changqing Guo,Guanghui Chen,Ning Wang,Shougui Wang,Yuwen Gao,Jipeng Dong,Qing Lu,Fei Gao
Several novel multifunctional histidine-based hypercrosslinked ionic polymers (HIPs) were constructed via a one-pot copolymerization strategy. The resultant HIPs were characterized by various technologies and investigated for the CO 2 adsorption and conversion. Plentiful hydrogen bond donors, nucleophilic ionic sites, and Lewis bases were successfully integrated into the HIPs skeletons. As-prepared histidine-based HIPs possess excellent hierarchical pore structure. The optimal HIP-Br-His exhibits a high CO 2 capture capacity of 2.90 mmol/g at 273 K and 1 bar, much higher than that of corresponding hypercrosslinked polymer HCP-Br without histidine units. Meanwhile, the HIP-Br-His achieves an excellent catalytic activity of 95 % product yield with 99 % product selectivity in CO 2 cycloaddition to propylene oxide under metal-, cocatalyst- and solvent-free and mild conditions (70 °C and 1.0 MPa). Particularly, HIP-Br-His can efficiently capture and convert dilute CO 2 into cyclic carbonates with a satisfactory catalytic performance. The excellent catalytic activity associating with the confirmed good stability, recyclability, and substrate compatibility make the developed histidine-based HIPs a promising heterogeneous catalyst for efficient CO 2 capture and conversion.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Menglei Mao,Ruqing Chong,Feixue Sun,Rui Gao,Zihui Meng,Xinlong Fan,Wenfang Liu
Enzymatic conversion of CO 2 to formate is a highly significant pathway for CO 2 utilization, but current level of conversion efficiency remains unsatisfactory due to low solubility of CO 2 under mild conditions. CO 2 -philic materials can significantly augment the reaction by raising local concentration of substrate. Herein, the intercalated Ti 3 C 2 T x , nano-silica (SiO 2 ) and carbon nitride (CN) with abundant CO 2 adsorption sites were introduced to fabricate Ti 3 C 2 T x based nanocomposites, Ti 3 C 2 T x /SiO 2 /CN (TSCN), for the first time. As the controls, binary composites including Ti 3 C 2 T x /SiO 2 (TS), Ti 3 C 2 T x /CN (TCN) and SiO 2 /CN (SCN) were also studied. For each kind of material, the composition, structure, morphology, and application performance in the enzymatic CO 2 conversion were characterized and influencing factors were investigated. Among these composites, TSCN exhibited the best application performance and the enzyme reaction was accelerated up to 23.9 times that of the blank system. The value could reach as high as 35.3 after polyethyleneimine (PEI) modification. Following that, PEI modified composites were used as carrier of formate dehydrogenase (FDH) and apparent specific activity was up to 2.8 times that of free enzyme, which could retain 88.2% of the initial value after 10 cycles associated with the structural integrity. This work provides new impetus to CO 2 capture and conversion in a clean and mild way that shows bright application prospects.
研究领域:
材料科学
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环境科学
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化学工程
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生物技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Ke-Ying Tao,Kuo Yuan,Wei Yang,Di-Chang Zhong,Tong-Bu Lu
Photocatalytic CO 2 reduction reaction (CO 2 RR) is an effective mean to address the current environmental and energy issues. As a kind of typical photocatalyst, g-C 3 N 4 possesses lots of advantages (i.e . , facile synthesis, visible-light response, and high stability) in CO 2 reduction. However, the poor capacity of CO 2 capture and rapid recombination of photo-generated electron and hole, both hinder the further development of g-C 3 N 4 for CO 2 RR. Herein, we developed a template co-pyrolysis strategy to prepare C–NH x -rich ( x = 1 or 2) g-C 3 N 4 , to increase the CO 2 binding and the subsequent photocatalytic CO 2 reduction efficiency. Specifically, organic molecules with multiple imino groups were used as additives to co-pyrolyze with urea. These additives can act as templates to facilitate the formation of g-C 3 N 4 with abundant C–NH x groups, which effectively improved the capacity of CO 2 capture. Meanwhile, the capacity of light absorption and the separation of photo-generated electron and hole were also optimized. As a result, the obtained C–NH x -rich g-C 3 N 4 showed greatly enhanced photocatalytic activity for CO 2 RR, over 74-fold higher than that of g-C 3 N 4 conventionally prepared. This work provides a new avenue for optimizing the g-C 3 N 4 -based photocatalysts for CO 2 RR.
研究领域:
材料科学
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环境科学
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能源科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
TEXTILE RESEARCH JOURNAL
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2022
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IF 2.455
Huizhen Ke,Qin Fang,Yitong Han,Huanda Zheng,Laijiu Zheng,Yuanyuan Dong
Traditional water-based flame-retardant finishing causes serious pollution due to the use of a large number of chemicals, and color change is easily generated since the flame-retardant finishing takes place after the cotton dyeing. An eco-friendly flame-retardant finishing of dyed cotton was explored using 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO), 2,2′-oxybis-(5,5-dimethyl-1,3,2,-dioxaphosphorinane-2,2′-disulfide) (5060), SiO2, DOPO/SiO2 (1:1), 5060/SiO2 (1:1) and DOPO/5060 (1:1) in supercritical CO2. The effects of finishing time and pressure as well as temperature on the flame-retarding properties of the cotton were discussed. As expected, samples with the higher weight gain rates exhibit a lower after-flame time as well as after-glow time. In different flame-retardant systems, cotton fabric finished with DOPO presents the lowest after-flame time of 20.6 s and after-glow time of 0 s at 130°C, 22 MPa and 120 min due to its biphenyl ring and O=P-O bond. Moreover, tiny fluctuations of L*, a*, b* and K/S values occurred from 32.10 to 34.24, 5.78 to 6.05, –37.89 to –37.64 and 10.59 to 10.81 when the cotton samples were treated with DOPO, 5060, SiO2, DOPO/SiO2 (1:1), 5060/SiO2 (1:1) and DOPO/5060 (1:1), proving that no significant negative role in the color property of the samples occurs after supercritical CO2 finishing.
研究领域:
纺织科学
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材料科学
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产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
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2025
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IF 5.6
Xu Ji,Weicong Xu,Chao Liu,Xing Wang
The electrocatalytic CO₂ reduction reaction (CO₂RR) offers a promising pathway for carbon cycling and high-value fuel synthesis. However, the efficient production of ethylene (C₂H₄), a critical multicarbon product, remains constrained by insufficient catalyst activity and selectivity. Although copper-based materials enable C–C coupling, conventional CuO catalysts suffer from imbalanced *CO intermediate adsorption strength and sluggish charge transfer kinetics.In this study, a silica (SiO₂) doping strategy was employed to synergistically modulate the electronic structure and surface active site distribution of CuO, significantly enhancing CO₂-to-C₂H₄ conversion efficiency. Experimental results demonstrate that SiO₂ incorporation induces local electronic density rearrangement around Cu²⁺, stabilizing *CO adsorption, while the constructed Cu-O-Si interfaces accelerate charge transfer, enhances electron transfer and reduce the energy barrier for *COCHO formation. The optimized SiO₂-10%/CuO catalyst achieves a C₂H₄ Faraday efficiency of 42% and a partial current density of 6.3 mA/cm² at −1.4 V (vs. RHE), representing a threefold improvement over pristine CuO. Notably, the catalyst exhibits exceptional stability over 4 hours.Structural characterization and theoretical calculations reveal that SiO₂ doping promotes the self-assembly of CuO nanosheets into flower-like architectures with a high specific surface area and exposes synergistic (111)/(002) facets, which collectively enhance *CO intermediate enrichment and directional coupling. This work provides novel insights into designing high-performance CO₂RR catalysts through multidimensional modulation strategies.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Meixue Zhao,Jianping Guo,Qingping Xin,Yanli Zhang,Xu Li,Xiaoli Ding,Lei Zhang,Lizhi Zhao,Hui Ye,Hong Li,Guangyu Xuan,Yuzhong Zhang
Membrane separation is a novel technology that has been widely studied for efficient CO 2 capture. This study aims to synthesize novel porous amino-functionalized nanosheets using PEI (polyethyleneimine) (PEI-F-Ce) and PEI-F-Ce/polyethylene oxide (PEO) mixed matrix membranes (MMMs). PEI-F-Ce nanosheets were prepared via the electrostatic self-assembly method, allowing for the adjustment of both lateral and pore sizes of the nanosheets by varying the PEI concentration. The MMMs loaded with 2 % PEI-F-Ce-2.5 nanosheets exhibit excellent CO 2 permeability (641 Barrer) and outstanding CO 2 /N 2 selectivity (70.1). These values surpassed those of pure PEO membranes by 62 % and 53 %, respectively, exceeding the 2019 upper bound. PEI-F-Ce-2.5 nanosheets with a stable pore channel 3.406 nm improved CO 2 transport and showed a large CO 2 adsorption capacity of 1.32 mmol g −1 , leading to enhanced the CO 2 /N 2 reaction selectivity. Moreover, the reversible reaction of CO 2 with –NH 2 enhanced the CO 2 /N 2 selectivity by 5.1 times at −20 °C, thereby highlighting its potential for cryogenic gas separation applications.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
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2022
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IF 5.436
Yimeng Zhou,Qianjin Ye,Xiangli Shi,Qiong Zhang,Qi Song,Changjian Zhou,Di Li,Deli Jiang
Due to the multiple electron and proton transfer processes involved, the photogenerated charges are easily recombined during the photocatalytic reduction of CO2, making the generation of the eight-electron product CH4 kinetically more difficult. Herein, Ni3B nanoparticles modulated by p-block element were combined with TiO2 nanosheets to construct a novel Schottky junction photocatalyst (Ni3B/TiO2) for the selective photocatalytic conversion of CO2 to CH4. The formed Ni3B/TiO2 photocatalyst with Schottky junction ensures a transfer pathway of photogenerated electrons from TiO2 to Ni3B, which facilitates the accumulation of electrons on the surface of Ni3B and subsequently improves the activity of photocatalytic CO2 reduction to CH4. The optimized Ni3B/TiO2 Schottky junction shows an improved CH4 yield of 30.03 μmol g–1 h–1, which was much higher than those of TiO2 (1.62 μmol g–1 h–1), NiO/TiO2 (2.44 μmol g–1 h–1), and Ni/TiO2 (4.3 μmol g–1 h–1). This work demonstrated that the introduction of p-block elements can alleviate the scaling relationship effect of pure metal cocatalysts to a certain extent, and the modified Ni3B can be used as a promising new cocatalyst to effectively improve the selective photocatalytic of CO2 to CH4.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
iScience
·
2025
·Vol. 28
·期 8
·113127
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IF 4.1
Chengzhuang Zhang,Jia Fang,Zhiqiang Han,Peng Chen,Xilong Xu,Kejian Wang,Yunxi Shi,Jianxiong Liao
CaO-based adsorbents present a promising approach for industrial CO 2 emissions reduction. This study systematically investigates the influence of adsorption temperature, adsorbent mass, CO 2 concentration, and flow rate on CO 2 capture efficiency using commercial CaO via thermogravimetric analysis (TGA). Optimal adsorption performance, achieving a capacity of 0.62 g/g and a rate exceeding 0.14 g/g/min, was observed at 750°C, 7 mg mass, 20% CO 2 , and 20 mL/min flow. Characterization (SEM, BET, and FTIR) indicated that 750°C preserved a hierarchical pore structure (24.64 m 2 /g surface area, 0.1026 cm 3 /g pore volume, and 7.08 nm average pore size), mitigating sintering and pore blockage while confining carbonation to surface layers. Kinetic modeling confirmed chemisorption dominance (pseudo-second-order). These findings elucidate fundamental mass/heat transfer limitations, supporting the development of enhanced CaO-based carbon capture, utilization, and storage (CCUS) technologies. Applied sciences; Chemistry; Environmental science.
研究领域:
应用科学
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化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Nature Catalysis
·
2025
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IF 44.6
Huang Liang,Gao Ge,Zhao Jiwu,Roberts William L.,Lu Xu
Electrochemical upcycling of captured CO 2 under high pressure holds significant potential to bridge between CO 2 emissions and hydrocarbon commodities, yet it remains underexplored. Here we convert gas-phase high-pressure captured CO 2 into ethylene (C 2 H 4 ) using a high-pressure membrane electrode assembly equipped with In/Cu catalysts, affording up to 85% Faradaic efficiency and 750 mA cm −2 partial current density under 20 bar. Theoretical calculations and operando studies link enhanced C–C coupling to the pressure-modulated *CO adsorption configuration and elevated CO 2 coverage. High pressure also mitigates salt precipitation by relocating bicarbonate formation to the catalyst–membrane interface, enabling stable electrolysis for over 1,500 h at 600 mA cm −2 . As a proof of concept, by recapturing residual CO 2 , the system delivers industrial-grade 99.9% purity C 2 H 4 , creating an opportunity to turn the otherwise costly CO 2 capture into a profit. Energy analysis suggests that directly valorizing high-pressure captured CO 2 , instead of depressurizing and repressurizing, is essential to minimize energy consumption.
研究领域:
电化学
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环境科学
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能量转化
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催化
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
Small
·
2023
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IF 13.3
Kai Zhang,Cuiping Xu,Xingjian Zhang,Zhiyi Huang,Qixiang Pian,Kunhong Che,Xiaokun Cui,Yueru Hu,Yimin Xuan
The chemical inertness of CO 2 molecules makes their adsorption and activation on a catalyst surface one of the key challenges in recycling CO 2 into chemical fuels. However, the traditional template synthesis and chemical modification strategies used to tackle this problem face severe structural collapse and modifier deactivation issues during the often-needed post-processing procedure. Herein, a CO 2 self-selective hydrothermal growth strategy is proposed for the synthesis of CeO 2 octahedral nanocrystals that participate in strong physicochemical interactions with CO 2 molecules. The intense affinity for CO 2 molecules persists during successive high-temperature treatments required for Ni deposition. This demonstrates the excellent structural heredity of the CO 2 self-selective CeO 2 nanocrystals, which leads to an outstanding photothermal CH 4 productivity exceeding 9 mmol h -1 m cat -2 and an impressive selectivity of >99%. The excellent performance is correlated with the abundant oxygen vacancies and hydroxyl species on the CeO 2 surface, which create many frustrated Lewis-pair active sites, and the strong interaction between Ni and CeO 2 that promotes the dissociation of H 2 molecules and the spillover of H atoms, thereby greatly benefitting the photothermal CO 2 methanation reaction. This self-selective hydrothermal growth strategy represents a new pathway for the development of effective catalysts for targeted chemical reactions.
研究领域:
材料科学
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）