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ENERGY CONVERSION AND MANAGEMENT · 2021 · IF 9.709

Facile synthesis of high-performance indium nanocrystals for selective CO2-to-formate electroreduction

Liangping Xiao,Xiao Liu,Renwu Zhou,Tianqi Zhang,Rusen Zhou,Bo Ouyang,Erjun Kan,Patrick J. Cullen,Kostya (Ken) Ostrikov,Xin Tu

Selective electrocatalytic reduction of CO 2 to formate has received increasing interest for CO 2 conversion and utilization. Yet, the CO 2 reduction process still faces major challenges, partly due to the lack of cost-effective, highly active, selective and stable electrocatalysts. Here, we report a mesoporous indium ( mp -In) electrocatalyst composed of nanobelts synthesized via a simple solution-based approach for selective CO 2 reduction to formate. The mp -In nanocrystals provide enlarged surface areas, abundant surface active sites and edge/low-coordinated sites. Such advantages afford the mp -In with an outstanding electrocatalytic performance for the CO 2 -to-formate conversion. A high formate selectivity, with a Faradaic efficiency (FE) of >90% was achieved over a potential of −0.95 V to −1.1 V ( vs V RHE ). The mp -In catalyst showed excellent durability, reflected by the stable formate selectivity and current density over a 24 h reaction period. Density functional theory (DFT) calculations reveal that the stabilization of the intermediate OCHO* on the In-plane surfaces is energetically feasible, further elucidating the origin of its enhanced CO 2 -to-formate activity and selectivity. This work may offer valuable insights for the facile fabrication of porous hierarchical nanostructures for electrocatalytic and selective reduction of CO 2 .

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CELLULOSE · 2020 ·Vol. 27 ·期 17 ·10541-10551 · IF 4.21

Reactive modified curcumin for high-fastness nonaqueous SC-CO2 dyeing of cotton fabric

Wang Mingyue,Liu Mao,Zhao Hongjuan,Xiong Xiaoqing,Zheng Laijiu

Abstract Modified curcumin, which has the advantages of low toxicity, high solubility, and little color change after modification, is very suitable for nonaqueous supercritical carbon dioxide cotton dyeing. However, the existing curcumin modification technology focuses on improving its solubility. Modified curcumin is directly adsorbed onto cotton fabrics, and the main interaction forces are van der Waals forces, which causes the poor fastness of modified curcumin to dyed cotton fabrics. In this study, reactive groups (hydroxyalkyls) were introduced into curcumin to enhance its fastness to cotton fabrics. The results showed that, similar to alkyl groups, hydroxyalkyl groups can enhance the color depth of dyed cotton fabrics by elevating the solubility of modified curcumin in supercritical carbon dioxide. The higher the solubility of modified curcumin in supercritical carbon dioxide was, the higher the K/S value of the dyed cotton fabric. Furthermore, the hydroxyl groups on the modified curcumin could form ether bonds with the hydroxyl groups on cotton fabrics. Therefore, the washing and rubbing fastness of hydroxyalkyl-curcumin-dyed cotton fabric was better than that of alkyl-curcumin-dyed cotton fabric. Graphic abstract

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CATALYSIS TODAY · 2024 · IF 5.2

The copper size effect of CuZn/CeO2 catalyst in CO2 hydrogenation to methanol

Lan Zhang,Xiaomin Hu,Ning Wang,Biaohua Chen

The escalating emission of CO 2 has caused a significant environmental impact. Hydrogenation of CO 2 to methanol stands as the primary objective in the liquid sunlight vision, aiming to mitigate CO 2 emissions. CuZn-based transition metal catalysts, known for their cost-effectiveness, demonstrate commendable catalytic performance at moderate temperatures and pressures, showcasing considerable potential in industrial applications. Consequently, a series of catalysts, composed of CuZn-based species supported on CeO 2 with strategically introduced appropriate oxygen vacancies, were meticulously prepared. It worth to noting that the size of Cu was precisely tuned, along with the enhanced ability to the adsorption and activation of CO 2 and H 2 . As a result, the optimal CuZn/CeO 2 catalyst exhibits high methanol formation rate, recording at 433.4 g MeOH kg cat −1 h −1 with selectivity of 68.5% at 260 °C and 3 MPa. Simultaneously, the reaction path and the evolution of intermediates in CO 2 hydrogenation was thoroughly delineated.

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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Rapid Homogeneous Acylation of Cellulose in a CO2 Switchable Solvent by Microwave Heating

Zongze Yao,Shu Mi,Bin Chen,Fei Liu,Haining Na,Jin Zhu

The acylation modification of cellulose to make it processable is an important method to utilize this green, renewable material with broad prospects. However, it usually takes several hours or even more than 20 h to obtain products with a high degree of substitution (DS) through the methods reported in the existing literature, especially for cellulose acetate (CA). In this study, rapid homogeneous acylation of cellulose is achieved in a novel CO2 switchable solvent system by using microwave heating. CA products with DS ranging from 1.83 to 2.91 can be obtained within 3–15 min by using acetic anhydride as the acylation reagent. This strategy can also be applied for the synthesis of a series of cellulose esters with different side chain lengths, and it takes only 10 min to produce cellulose esters with a DS higher than 2.20 under microwave heating. This study suggests a facile and effective method for the synthesis of cellulose esters.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Tungsten-doped high-silica CHA zeolite membranes with improved hydrophobicity for CO2 separation

Li Peng,Zhaofeng Duan,Shumin Cen,Xuehong Gu

High-silica CHA (SSZ-13) zeolites membranes, with pore size between the molecular size of CO 2 and N 2 or CH 4 , are promising for some industrial CO 2 separation process. Considering water is typically present in these industrial gas feed and the negative impact of moisture on the membranes’ gas permeation, it is highly desirable to increase the surface hydrophobicity of membranes to reduce the adsorption of water. In this paper, a W-doping strategy was proposed to increase the hydrophobicity of SSZ-13 membranes by eliminating the silanols on the surface, and the W-doped high-silica CHA (W-SSZ-13) zeolite membranes were prepared for the first time. Characterizations such as SEM, XRD, and XPS confirmed the successful incorporation of W into CHA membrane. The incorporation of W reduced the pore mouth size, and the W-SSZ-13 zeolite membranes showed improved CO 2 /N 2 and CO 2 /CH 4 separation performance. After W-doping, the maximum separation factors ( α max ) for the CO 2 /N 2 mixture with equimolar composition under dry conditions increased from 8.8 to 16.9, and for the equimolar CO 2 /CH 4 mixture, the value increased from 105.9 to 176. The W-SSZ-13 membranes also showed better separation performance under wet conditions. For both systems, the W-SSZ-13 membrane showed higher α max and less CO 2 permeance reductions, indicating a more resistance in wet conditions.

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CHEMIE INGENIEUR TECHNIK · 2021 · IF 1.672

CO2-Philic Mixed-Matrix Membranes Based on Ultra-Stable Porous-Framework Zirconium Phosphate

Taotao Ji,Liangliang Liu,Lingyi Wang,Yanshuo Li,Yi Liu

The practical application of membrane separation, such as CO 2 recovery from flue gas, is usually accompanied by harsh operating conditions of high temperature and pressure as well as acidic and humid feed properties, which poses a great challenge to the stability of membrane materials. In this work, zirconium phosphate material with highly stable porous-framework structure was synthesized by ionothermal method, and then, its incorporation into the polymer matrix to prepare ZrPOF-Pebax mixed-matrix membranes (MMMs) was pioneered. Benefiting from their 4.0 × 3.0 Å 7-ring windows and CO 2 -philic framework, the optimal MMMs with a 5 wt % ZrPOF content exhibited enhanced CO 2 /N 2 selectivity of 29.6, with a decent CO 2 permeability of 286.3 Barrer, which raised by 79.4 and 67.5% compared to the neat Pebax 2533 membranes, respectively. Furthermore, owing to their excellent thermal, water, and chemical stability, obtained MMMs maintained excellent performances under harsh operating conditions.

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CARBON · 2019 · IF 7.466

Cubic Cu2O on nitrogen-doped carbon shells for electrocatalytic CO2 reduction to C2H4

Hui Ning,Xiaoshan Wang,Wenhang Wang,Qinhu Mao,Zhongxue Yang,Qingshan Zhao,Yan Song,Mingbo Wu

Electroreduction of carbon dioxide (CO 2 ) to ethylene (C 2 H 4 ) is one of the most feasible approaches to reduce the carbon emissions and enhance carbon dioxide utilization , whereas the lack of efficient catalysts impedes the scale application. Cuprous oxide (Cu 2 O) is a promising catalyst for the formation of C 2 H 4 but with unsatisfied selectivity and stability. Herein, we prepared Cu 2 O/nitrogen-doped carbon shell (Cu 2 O/NCS) composite and employed it in the production of C 2 H 4 from CO 2 electroreduction. The ultra-thin NCS with graphene-like structure was prepared from petroleum asphalt by template method . The cubic Cu 2 O nanocrystals are uniformly dispersed on the surface of NCS with ca. 150 nm diameters. Cu 2 O/NCS loaded on glass carbon electrode showed a high faradaic efficiency of C 2 H 4 (24.7%) at −1.3 V ( vs . reversible hydrogen electrode) as well as remarkable stability. The excellent performance of Cu 2 O/NCS is attributed to the high dispersion of cubic Cu 2 O nanocrystals and the abundant pyridinic-N moieties in NCS. This work provides a new strategy to improve the selectivity and durability of Cu 2 O for production C 2 H 4 from electrocatalytic CO 2 reduction by fabricating composites with nitrogen-doped carbon materials.

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PROCESS BIOCHEMISTRY · 2015 · IF 2.516

Immobilization of carbonic anhydrase on epoxy-functionalized magnetic polymer microspheres for CO2 capture

Guohua Jing,Fujun Pan,Bihong Lv,Zuoming Zhou

Carbonic anhydrase (CA) is the most efficient catalyst for CO 2 hydration and dehydration. In the present work, magnetic polymer microspheres functionalized with epoxy group were prepared, and CA enzyme was immobilized on the carries by selective covalent binding. The parameters affecting CA immobilization, such as pH, temperature and enzyme dose were investigated. Based on the investigation and the characterization of the microspheres, the kinetic parameters of the immobilized and the free CA were also evaluated. The value of the Michaelis–Menten constant ( K m ) and the maximum velocity ( V max ) of the immobilized CA was 8.077   mmol/L (mM) and 0.027   μmol/(min   mL), while that of the free CA was 6.091   mM and 0.091   μmol/(min   mL), respectively. Moreover, the performance of the thermal stability, storage stability and reusability of the immobilized CA confirmed that CA immobilized on the epoxy-functionalized magnetic polymer microspheres owned a stable and efficient catalytic ability on CO 2 hydration, which seemed to be a suitable candidate for CO 2 capture.

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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Synergy of oxygen vacancy and piezoelectricity effect promotes the CO2 photoreduction by BaTiO3

Weihua Cai,Xinyu Ma,Jin Chen,Ruochen Shi,Yabo Wang,Yawei Yang,Dengwei Jing,Hudie Yuan,Jing Du,Meidan Que

Great efforts have been devoted to developing efficient visible-light-driven photocatalysts for the conversion CO 2 into clean fuels. Nevertheless, the photoreduction of CO 2 is hampered by inadequate surface-active sites and ineffective electron-hole pair separation. Herein, we explore the wheat-heading BaTiO 3 with high surface area and piezoelectricity to facilitating their bulk charge separation. Meanwhile, oxygen vacancies were fabricated to extending the visible light absorption range and increasing the active sites of the wheat-heading BaTiO 3 , thus promoting the photocatalytic performance of CO 2 . Among the wheat-heading BaTiO 3 -X (X = 0, 0.5, 1.0, 1.5, 2.0) catalysts, BaTiO 3 -1.5 affords the optimal photocatalytic performance of CO, 6.41 μmol·g −1 under light, 9.17 μmol·g −1 under light and ultrasound, which were 3.22 and 1.86 times higher for pristine wheat-heading BaTiO 3 , respectively. This synergetic strategy sheds a new light on piezoelectric properties and surface defect engineering, while emphasizing the importance of surface properties in enhancing CO 2 conversion performance.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

A chemically stable La0.2Sr0.8Fe0.9Mo0.1O3-δ-molten carbonate dual-phase membrane for CO2 separation

Shipeng Zeng,Zilu Liu,Hailei Zhao,Tianrang Yang,Xu Dong,Zhihong Du

We report here a mixed oxygen ionic-electronic conductor-molten carbonate composite membrane for high temperature CO 2 separation. Mo-doping at Fe-site of La 0.2 Sr 0.8 FeO 3-δ (LSF) is attempted to address its stability issue in CO 2 or carbonate-containing environment. The La 0.2 Sr 0.8 Fe 0.9 Mo 0.1 O 3-δ (LSFM)-molten carbonate membrane with 1 mm thickness delivers a CO 2 permeation flux of 1.57 × 10 −3 mol m −2 s −1 at 800 °C with 50% CO 2  + 50 % N 2 (total 1 atm) as feeding gas and pure He (1 atm) as sweeping gas, compared to 0.737 × 10 −3 mol m −2 s −1 for the LSF counterpart. The CO 2 permeation flux further increases to 2.25 × 10 −3 mol m −2 s −1 for membrane prepared with Al 2 O 3 coated LSFM substrate. An even higher CO 2 permeability of 2.69 × 10 −3 mol m −2 s −1 is demonstrated for LSFM-molten carbonate membrane at 800 °C when using simulated flue gas (15% CO 2  + 10% O 2  + 75 % N 2 in total 1 atm) as feeding gas. The membrane also exhibits relatively stable CO 2 and O 2 fluxes during 50 h test at 750 °C. The designed LSFM-molten carbonate membrane can be potentially used as a reactor for dry methane reforming and partial oxidation of methane with flue gas as direct feedstock.

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APPLIED ORGANOMETALLIC CHEMISTRY · 2015 ·Vol. 29 ·期 4 ·240-243 · IF 2.248

Cycloaddition of epoxide and CO2 to cyclic carbonate catalyzed by VO(IV) porphyrin

Dongsheng Bai,Zhiyong Zhang,Guangjian Wang,Fang Ma

The cycloaddition of epoxide and CO 2 to synthesize cyclic carbonate catalyzed by VO(IV) porphyrin was achieved under 1.4 MPa at 150°C. The effects of reaction temperature, time, CO 2 pressure, co-catalyst and porphyrin framework were investigated. The catalytic results showed that moderate to high yields of cyclic carbonates were obtained under the optimal reaction conditions. Copyright © 2015 John Wiley & Sons, Ltd.

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Green Energy & Environment · 2017 · IF 0

Synthesis of polyurea from 1,6-hexanediamine with CO2 through a two-step polymerization

Shan Jiang,Ruhui Shi,Haiyang Cheng,Chao Zhang,Fengyu Zhao

Activation and transformation of CO 2 is one of the important issues in the field of green and sustainable chemistry. Herein, CO 2 as a carbon-oxygen resource was converted to CO 2 -polyurea with 1,6-hexanediamine through a two-step polymerization. The reaction parameters such as temperature, pressure and reaction time were examined; and several kinds of catalysts were screened in the absence and presence of NMP solvent. The formed oligomer and the final polyurea were characterized by FT-IR, VT-DRIFTS, NMR, XRD, AFM and their thermal properties were examined by TGA and DSC. It was confirmed that the final polyurea has a high thermal stability; the melting temperature is 269 °C and the decomposition temperature is above 300 °C. It is a brittle polymer with a tensile strength of 18.35 MPa at break length of 1.64%. The polyurea has a stronger solvent resistance due to the ordered hydrogen bond in structure. The average molecular weight should be enhanced in the post-polymerization as the appearance, hydrogen bond intensity, crystallinity, melting point and the thermal stability changed largely compared to the oligomer. The present work provides a new kind of polyurea, it is expected to have a wide application in the field of polymer materials.

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