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FUEL PROCESSING TECHNOLOGY · 2024 · IF 7.2

Synergistic promotions between high purity H2 production and CO2 capture via sorption enhanced chemical looping reforming

Mingkai Liu,Yang Li,Xuyun Wang,Zhongrui Gai,Qiong Rao,Tianlong Yang,Jinrui Zhang,Sanli Tang,Ying Pan,Hongguang Jin

Hydrogen energy, a promising clean source, holds potential to combat global warming. To achieve efficient and low-carbon H 2 production, we proposed an isothermal sorption-enhanced chemical looping reforming (SE-CLR) process to realize the high-purity hydrogen production and in-situ CO 2 capture at mild temperatures (550–650 °C). For practical application, the process is characterized to use Fe-Ni double metal oxide particles as steam methane reforming oxygen carriers, and K 2 CO 3 -promoted Li 4 SiO 4 particles as CO 2 sorbent. The oxygen transfer capacity of metal oxide matintained high at 57.4%, and the K-Li 4 SiO 4 absorbents remained at 22.5% CO 2 absorption capacity over 200 isothermal absorption-regeneration cycles. Conducting a synergistic conversion mechanism within double metal oxides and absorbents, and adjusting the absorbent-to-metal oxide mass ratio to 7:4, enhanced hydrogen purity to 92% and CO 2 uptake to 95%. Furthermore, in-situ CO 2 removal in CLR processes achieved methane conversion and H 2 production rates equivalent to conventional CLR processes under the same reaction conditions, but at temperatures ∼60 °C lower. The effects of the reaction temperature, pressure, steam-to-methane and methane-to-solid ratios on SE-CLR performance were studied systematically. Finally, stable hydrogen production with a purity of 91%–89% and CO 2 uptake of 94%–91% were obtained over 25 CLR cycles, with minimal changes in mechanical strength of particles.

✓ 已验证 DOI 高影响因子
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Cell Reports Physical Science · 2022 · IF 7.832

Fabrication of long-life quasi-solid-state Na-CO2 battery by formation of Na2C2O4 discharge product

Bowen Xu,Da Zhang,Shilei Chang,Minjie Hou,Chao Peng,Dongfeng Xue,Bin Yang,Yong Lei,Feng Liang

Rechargeable Na-CO 2 batteries are promising energy-storage devices due to their high energy density, environmental friendliness, and cost effectiveness. However, the insulating nature and irreversibility of the Na 2 CO 3 discharge product cause large polarization and poor cyclicity. Here, we report a reversible quasi-solid-state Na-CO 2 battery that is constructed by the synergistic action of a Co-encapsulated N-doped carbon framework catalyst and gel electrolyte to ensure the formation of a highly reversible Na 2 C 2 O 4 discharge product. Experiments and density functional theory calculations indicate that the electron-agglomeration effect of Co nanoparticles enhances CO 2 adsorption and lowers energy barrier, as well as promotes Na 2 C 2 O 4 generation. A gel electrolyte containing an imidazole organic cation is used to inhibit the decomposition of the thermodynamically unstable Na 2 C 2 O 4 . The fabricated Na-CO 2 battery exhibits a high discharge capacity of 3,094 mAh g −1 , a high-rate performance of 1,777 mAh g −1 at a current density of 0.5 mA cm −2 , and excellent cycling performance of 366 cycles (2,200 h).

✓ 已验证 DOI 高影响因子
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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2020 ·Vol. 221 ·期 13 ·2000145 · IF 2.335

Preparation of Polyurethane-Urea Elastomers Using Low Molecular Weight Aliphatic Diamines Enabled by Reversible CO2 Chemistry

Bo Zhang,Xiaoxiao Li,Yumeng Tian,Jie Wang,Xiaoli Zhao,Xiaoniu Yang

The use of low molecular weight (LMw) aliphatic diamines for the synthesis of polyurethane-urea elastomers (PUUEs) is an effective method for introducing abundant, strong hydrogen bonds with the aim of improving the thermal and mechanical properties of PUUEs. However, the reaction between isocyanates and LMw aliphatic diamines is too rapid to produce PUUEs. In this study, PUUEs incorporating LMw aliphatic diamines as chain extenders are prepared via the reversible reaction of CO 2 with diamines. The phase separation, thermal properties, and thermomechanical and mechanical properties of polyurethane materials are investigated as the chain extender changed from diol to diamine. Replacing the diol chain extenders with diamine results in the formation of more abundant and stronger hydrogen bonds in PUUEs, which enables the assembly of long range ordered structures and improved microphase separation. The tensile strengths of PUUEs, from 8.4 to 13 MPa, are much higher than their corresponding polyurethanes, owing to the physical crosslinks formed by the more and stronger hydrogen bonds in the PUUEs.

✓ 已验证 DOI 高影响因子
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2022 · IF 3.898

Covalent organic frameworks-incorporated thin film composite membranes prepared by interfacial polymerization for efficient CO2 separation

Haoqing Xu,Wenyan Feng,Menglong Sheng,Ye Yuan,Bo Wang,Jixiao Wang,Zhi Wang

Thin film composite (TFC) membranes with nanofillers additives for CO 2 separation show promising applications in energy and environment-related fields. However, the poor compatibility between nanofillers and polymers in TFC membranes is the main problem. In this work, covalent organic frameworks (COFs, TpPa-1) with rich NH groups were incorporated into polyamide (PA) segment via in situ interfacial polymerization to prepare defect-free TFC membranes for CO 2 /N 2 separation. The formed covalent bonds between TpPa-1 and PA strengthen the interaction between nanofillers and polymers, thereby enhancing compatibility. Besides, the incorporated COFs disturb the rigid structure of the PA layer, and provide fast CO 2 transfer channels. The incorporated COFs also increase the content of effective carriers, which enhances the CO 2 facilitated transport. Consequently, in CO 2 /N 2 mixed gas separation test, the optimal TFC (TpPa 0.025 -PIP-TMC/mPSf) membrane exhibits high CO 2 permeance of 854 GPU and high CO 2 /N 2 selectivity of 148 at 0.15 MPa, CO 2 permeance of 456 GPU (gas permeation unit) and CO 2 /N 2 selectivity of 92 at 0.5 MPa. In addition, the TpPa 0.025 -PIP-TMC/mPSf membrane also achieves high permselectivty in CO 2 /CH 4 mixed gas separation test. Finally, the optimal TFC membrane showes good stability in the simulated flue gas test, revealing the application potential for CO 2 capture from flue gas.

✓ 已验证 DOI 高影响因子
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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Effect of In(OH)3 species modified ZnS on improved photocatalytic activity of photoreduction of CO2

Qiao Zhao,Hanbo Li,Yaan Cao

A series of the In(OH) 3 species modified ZnS (ZnS–In(OH) 3 X% (X ​= ​2, 5, 7, 10)) photocatalysts were synthesized by a hydrothermal method . ZnS–In(OH) 3 X% (X ​= ​2, 5, 7, 10) exhibited the improvement of photocatalytic activity for the photoreduction of CO 2 into CO compared with ZnS. Characterized by X-ray diffraction (XRD), fourier transforms infrared spectra (FT-IR), high resolution transmission electron microscope (HRTEM), X-ray photoelectron spectroscopy (XPS) valence band spectra, UV–vis diffuse reflectance spectra, photoluminescence (PL) and time-resolved PL decay curves, the crystal structure, band structure and behaviors of photogenerated charge carriers for photocatalyst were explored up. It was revealed that the modification of In(OH) 3 surface species on surface of ZnS can prolong the fluorescence lifetimes of photogenerated charge carriers, enhance the separate of photoinduced charge carriers efficiently and promote better matching between the band structure and the redox potential of the CO 2 /CO, resulting in improvement of photocatalytic activity efficiently for ZnS–In(OH) 3 X% (X ​= ​2, 5, 7, 10) photocatalysts . This work may offer a new understanding to study the effect of surface species modification on photocatalytic performance of photocatalyst.

✓ 已验证 DOI 高影响因子
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JOURNAL OF POROUS MATERIALS · 2024 ·Vol. 31 ·期 3 ·897-912 · IF 2.5

MCM-41 supported quaternary ammonium ionic liquids as an effective heterogeneous catalyst for CO2 cycloaddition reaction

Lu Qing,Wang Shougui,Ji Cailin,Chen Guanghui,Dong Jipeng,Gao Fei

Ionic liquid immobilization is an effective means for preparing metal-free heterogeneous catalysts for the CO 2 conversion. Herein, a series of quaternary ammonium ionic liquids functionalized MCM-41 heterogeneous catalysts, integrating hydrogen bond donors and nucleophilic ion sites, were prepared by a post-synthetic modification method for the CO 2 cycloaddition reaction. The physicochemical properties of the catalysts were analyzed by XRD, EA, SEM, TEM, BET, FT-IR, TGA, NMR and XPS. The results show that the quaternary ammonium ionic liquids are successfully immobilized onto the MCM-41 molecular sieves. The obtained catalysts maintain an excellent pore structure and have the good thermal stability. The effects of catalytic conditions on the catalytic performance, the recyclability of the catalysts and their generalizability to epoxide substrates were systematically investigated. In addition, the catalytic performance was evaluated for low concentrations of CO 2 (20% CO 2 , 80% N 2 ). The synergy of multifunctional active sites makes the obtained materials exhibit the high catalytic activity without metals, co-catalysts and solvents. Furthermore, a possible mechanism for the conversion of CO 2 to cyclic carbonate catalyzed by the MCM-41-N/CH 3 (1:3) was proposed.

✓ 已验证 DOI 高影响因子
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2023 ·Vol. 170 ·期 5 ·053503 · IF 3.9

Simple and Controllable Preparation of Molybdenum Carbides by One-Step Co-Electrolysis of Na2MoO4 and CO2

Tao Wu,Jintao Zhang,Yunfei Chen,Yongzheng Jia,Jialiang An,Jianbang Ge,Mingyong Wang

Molybdenum carbides are the promising ceramic materials and catalysts. A new and green method for the controllable preparation of molybdenum carbides was proposed by one-step co-electrolysis of Na2MoO4 and CO2 greenhouse gas in carbonate molten salts. The solubility and decomposition thermodynamics of Na2MoO4 were analyzed. The structure, composition, current efficiency, energy consumption and extraction ratio of molybdenum carbide were effectively regulated by changing the molten salt composition, electrolytic voltage, temperature, and electrolytic time. It was confirmed that MoC, Mo2C or dual-phase MoC-Mo2C can be controllably prepared. Molybdenum carbides may be mainly obtained by the thermal reaction between C from CO2 and Mo from Na2MoO4. Molybdenum carbides prepared at 850 °C and 4.5 V in Na2CO3-K2CO3−32 wt% Li2CO3−15 wt% Na2MoO4 molten salts showed the best electrocatalytic activity for hydrogen evolution reaction. The work provides an innovative and sustainable strategy to prepare molybdenum carbides and utilize CO2.

✓ 已验证 DOI 高影响因子
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CATALYSIS COMMUNICATIONS · 2019 · IF 3.674

Photothermal reverse-water-gas-shift over Au/CeO2 with high yield and selectivity in CO2 conversion

Bowen Lu,Fengjiao Quan,Zheng Sun,Falong Jia,Lizhi Zhang

Photothermal reverse-water-gas-shift is realized with high conversion rate and selectivity of CO in the case of Au/CeO 2 catalyst. Moreover, photothermal reaction rate is much higher (>10 times) than that performed under thermal condition. As indicated by the results of in-situ infrared spectroscopy and kinetic experiments, the special role of light is found to be related with the promotion of hydrogen-splitting step. The robust Au/CeO 2 catalyst exhibits stable activity and CO selectivity under long-term light irradiation. It is expected that the combination of catalysts and light may afford new perspectives for the CO 2 hydrogenation.

✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2016 · IF 5.557

Facilitated transport membranes by incorporating graphene nanosheets with high zinc ion loading for enhanced CO2 separation

Dongdong Peng,Shaofei Wang,Zhizhang Tian,Xingyu Wu,Yingzhen Wu,Hong Wu,Qingping Xin,Jianfeng Chen,Xingzhong Cao,Zhongyi Jiang

In this study, a novel kind of facilitated transport membrane was prepared by incorporating zinc ion-modified graphene (GO-DA-Zn 2+ ) nanosheets into a poly(ether-block-amide) (Pebax) matrix. Graphene oxide (GO) nanosheets were modified with zinc ion (Zn 2+ ) by using dopamine-mediated complexation reaction. The CO 2 separation properties of the facilitated transport membrane were evaluated using CO 2 /CH 4 mixture as model system. The GO-DA-Zn 2+ nanosheets played an important role in enhancing membrane performance. First, the high zinc ion loading (34.2   wt% of the nanosheets) could enhance the facilitated transport of CO 2 based on π-complexation mechanism, leading to a higher CO 2 permeability and selectivity. Second, the incorporation of graphene nanosheets with high aspect ratio rendered more tortuous gas transport channels, which was favorable for hindering the penetration of CH 4 with larger molecular size and thus enhancing the CO 2 /CH 4 selectivity. Third, the fractional free volume of hybrid membrane was much elevated, also leading to higher CO 2 permeability. The optimum separation properties of GO-DA-Zn 2+ incorporated Pebax membranes were achieved with a CO 2 permeability of 137.9   Barrer and a CO 2 /CH 4 selectivity of 30.6, which were 49% and 78% higher than those of pristine Pebax membrane.

✓ 已验证 DOI 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Amino-functionalized NUS-8 nanosheets as fillers in PIM-1 mixed matrix membranes for CO2 separations

Yunchuan Pu,Ziqi Yang,Vanessa Wee,Zhongjie Wu,Zhongyi Jiang,Dan Zhao

Membrane-based separation technologies are promising for various applications such as carbon capture and storage (CCS). Herein, we report the preparation and performance of mixed matrix membranes (MMMs) for carbon dioxide (CO 2 ) separation. The MMMs comprise amino-functionalized metal-organic framework (MOF) nanosheets (NUS-8-NH 2 ) dispersed in the polymer of intrinsic microporosity 1 (PIM-1). Specifically, the MOF nanosheets were synthesized through a bottom-up method and introduced into the PIM-1 matrix to fabricate NUS-8-NH 2 /PIM-1 MMMs. The uniformly dispersed MOF nanosheets could afford additional fast transport pathways through intra-flake pores and inter-flake nano-channels. Moreover, the amino groups could enhance CO 2 transport within NUS-8-NH 2 /PIM-1 MMMs. In addition, hydrogen bonding between the NUS-8-NH 2 filler and PIM-1 matrix improved interfacial compatibility. Therefore, the as-prepared MMMs could achieve a high filler loading of 15 wt% without sacrificing separation performance. Compared with the pure PIM-1 membrane, the MMM with 10 wt% NUS-8-NH 2 showed CO 2 permeability of ∼14000 Barrer and a CO 2 /N 2 selectivity of ∼30, surpassing the 2008 Robeson's upper bound.

✓ 已验证 DOI 高影响因子
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2021 · IF 2.694

New Vapor–Liquid Phase Equilibrium Data of CO2 in Several Heavy n-Alkanes at High Pressures

JinTao He,XueMan Xu,Xia Gui

New phase equilibrium data of CO2 in n-hexadecane, n-heptadecane, n-octadecane, n-nonadecane, and n-eicosane were measured at temperatures from 333.15 to 373.15 K up to 23.73 MPa by a constant-volume method. Thermodynamic properties of Gibbs free energy (ΔsolG), enthalpy change (ΔsolH), entropy change (ΔsolS), and Henry’s coefficient (H) were calculated and analyzed for elucidating the dissolution mechanism of CO2 in alkanes. Results showed that the CO2 solubility increased with increasing pressure but decreased with increasing temperature and carbon number. In addition, increasing carbon number also led to an increase in the minimum miscibility pressure (MMP) of alkanes with CO2 and thus limited CO2 solubility in alkanes.

✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING SCIENCE · 2026 · IF 5.1

Advanced oxidation pretreatment of biomass for preparation of carbon-based adsorbents with high CO2 capture performance

Hongkai Di,Guangzhe Zhang,Hanrui Ma,Tong Hao,Zimeng Han,Jiangze Han,Jiao Liu,Fang Wang

The FeSO 4 ·7H 2 O/K 2 S 2 O 8 advanced oxidation system was adopted to prepare biochar-based CO 2 adsorbents. • The as-prepared adsorbent exhibited a high specific surface area of 1909.9 m 2 /g and a micropore ratio of 91.8 %. • The optimized adsorbent achieved a dynamic CO 2 adsorption capacity of 166.2 mg/g at 0 °C and 1 bar. • Advanced oxidation cut activator dosage and synergistically optimized microporous structure and surface chemistry. The advanced oxidation system composed of FeSO 4 ·7H 2 O/K 2 S 2 O 8 was adopted to pretreat pear tree branches, before carbonization and KOH activation, successfully producing porous carbon materials with excellent CO 2 adsorption performance. The sulfate radicals ( S O 4 - ∙ ) produced in the pretreatment process were capable of effectively breaking the chemical bonds between cellulose, hemicellulose, and lignin, leading to a decrease in the degree of polymerization. Concurrently, they convert the raw biomass into a loose, rough, lamellar architecture, accompanied with abundant oxygenic functional groups introduced. Dynamic adsorption tests confirmed the superior performance of ZBH@0.10, which delivered a CO 2 uptake of 166.1 mg/g at 0 °C, 124.8 mg/g at 25 °C and 98.3 mg/g at 45 °C under 0.1 MPa; static adsorption further revealed a CO 2 adsorption of 202.44 mg/g (25 °C, single–component isotherm) and a favorable CO 2 /N 2 selectivity of 30.24. After 10 regeneration cycles, the material maintained 98.7 % of its initial adsorption capacity, demonstrating excellent cycling stability. Mechanistic analysis indicated that physical adsorption played a primary role in the uptake process, with pore filling playing a key role. The pretreatment strategy significantly reduced the amount of activator required, while achieving synergistic optimization of the microporous structure and surface chemical properties and also markedly enhanced the CO 2 adsorption performance of the resulting adsorbent. This approach provided a new route for the resource utilization of agricultural and forestry wastes, as well as technological foundation for the design of low-cost, high-capacity biochar-based CO 2 sorbents.

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