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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

N, P co-doped cellulose-based carbon aerogel: A dual-functional porous material for CO2 capture and supercapacitor

Jian Yu,Jianfei Xiao,Yuan Wang,Tian C. Zhang,Ji Li,Ge He,Shaojun Yuan

Biomass-derived carbon aerogels have attracted considerable attention for applications in CO 2 capture and supercapacitors (SCs). However, these carbon aerogel materials often suffer from an insufficient number of active sites. In this study, a novel N, P co-doped porous carbon aerogel with a hierarchical structure was synthesized using cellulose biomass as the raw material, a NaOH/urea system as the solvent and activator, and urea and urea phosphate as heteroatom dopants. Owing to the synergistic effects of heteroatom co-doping and the hierarchical pore structure, the optimal sample, NPCA-600–0.5, exhibited a large specific surface area of 582.9 m 2 /g and a high pore volume of 0.187 cm 3 /g. It demonstrated a CO 2 adsorption capacity of 2.89 mmol/g (25 °C, 1 bar), along with high CO 2 /N 2 selectivity and excellent recyclability, retaining 91 % efficiency after 10 cycles. As a SC electrode, NPCA-600–0.5 achieved a high specific capacitance of 238 F/g at 1 A/g, maintaining 80 % of its initial capacitance after 5000 cycles at 10 A/g. This work not only provides a promising adsorbent and electrode material for CO 2 capture and supercapacitors, but also offers valuable insights for the design of advanced carbon-based materials.

CAS / MDL: 9004-34-6
研究领域: 材料科学 · 环境科学 · 能源存储
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APPLIED ENERGY · 2018 · IF 7.9

Evaluating CO2 desorption performance in CO2-loaded aqueous tri-solvent blend amines with and without solid acid catalysts

Xiaowen Zhang,Rui Zhang,Helei Liu,Hongxia Gao,Zhiwu Liang

To enhance the energy efficiency of the CO 2 desorption process, the regeneration behaviors of the CO 2 -loaded 6 M MEA-AMP-PZ (monoethanolamine, 2-amino-2-methyl-1-propanol and piperazine) tri-solvent blends with different AMP/PZ molar ratios with four different solid acid catalysts (H-ZSM-5, γ-Al 2 O 3 , SAPO-34 and SO 4 2− /TiO 2 ) and a blank at 96 °C were investigated in terms of CO 2 desorption rate, cyclic capacity and relative heat duty. For the no-catalytic runs, the results showed that all the tri-solvent blended amines greatly increased CO 2 desorption rate, cyclic capacity and decreased the relative heat duty in comparison with 5 M MEA. The 13 C NMR analysis indicated that the 3 M MEA-2.5 M AMP-0.5 M PZ blend with the highest AMP/PZ ratio produced the largest amount of bicarbonate and less carbamate, which resulted in the best desorption performance. With regard to catalyst, when the solid acid catalysts were introduced, the regeneration performance of the blend was further improved. The best of the blends along with H-ZSM-5 provided the combination with the best performance in CO 2 desorption, and reduced the relative heat duty by 61.6% as compared to 5 M MEA without catalyst (100%). Five relevant physicochemical properties of the catalyst were obtained and used to better understand the catalytic regeneration process. A possible catalytic CO 2 desorption mechanism was analyzed. The results revealed that the mesopore surface area coupled with total acid sites of the catalyst had the most positive influence on improving the CO 2 desorption performance. Findings from this work imply that the combination of solid acid catalyst with tri-solvent blended amines is a promising alternative method for further reduction of solvent regeneration energy requirement.

研究领域: 化学工程 · 环境科学
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APPLIED ENERGY · 2018 · IF 7.9

Reducing energy consumption of CO2 desorption in CO2-loaded aqueous amine solution using Al2O3/HZSM-5 bifunctional catalysts

Xiaowen Zhang,Helei Liu,Zhiwu Liang,Raphael Idem,Paitoon Tontiwachwuthikul,Mohammed Jaber Al-Marri,Abdelbaki Benamor

The aim of this work is to find a potential way for great decrease in CO 2 capture energy requirement. Here, for the first time, a series of bifunctional Al 2 O 3 /HZSM-5 catalysts (Al-ZSM) were prepared by the combined precipitation ultrasound method and used for the CO 2 desorption process. All the investigated catalysts were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrometry (FT-IR), N 2 adsorption–desorption, ammonia and CO 2 temperature programmed desorption (NH 3 /CO 2 -TPD) and pyridine-adsorption infrared spectroscopy (Py-IR). The regeneration behaviors of a 5 M monoethanolamine (MEA) solvent with four Al-ZSM catalysts were studied at an initial CO 2 loading of 0.5 mol CO 2 /mol amine and the temperature of 96 °C. The results reveal that all the catalysts improve the CO 2 desorption performance, the Al-ZSM catalysts show higher catalytic performance than the single catalysts Al 2 O 3 and HZSM-5, and the Al-ZSM can reduce the heat duty by 23.3–34.2% as compared with the catalyst-free test. The use of Al-ZSM in the MEA regeneration process improves the desorption performance by 2–3 times in comparison with the blank run. A possible dual sites mechanism of CO 2 desorption with Al-ZSM is suggested. The excellent performance of Al-ZSM can be attributed to their enhanced Brϕnsted acid sites (BAS), mesopore surface area (MSA) and basic sites, which resulted from the good synergistic reaction between the Al 2 O 3 and HZSM-5, and the base treatment for HZSM-5. Besides, the stability test of the Al-ZSM was conducted. Based on the results, the Al-ZSM demonstrate a superior catalytic performance for the rich amine regeneration process, and present an excellent cyclic stability, explicitly have the potential to be a promising industrial catalyst for CO 2 capture. Furthermore, the dual sites catalytic CO 2 desorption over bifunctional catalysts will open a new path to design better catalysts for the rich amine solution regeneration process to increase the desorption performance, reduce the regeneration energy consumption, and thus further decreasing the operation costs of CO 2 capture.

CAS / MDL: 1336-21-6 142-58-5
研究领域: 化学工程 · 环境科学
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

A green route to CO2 adsorption on biomass chitosan derived nitrogen-doped micropore-dominated carbon nanosheets by different activators

Jinhao Li,Agula Bao,Junxiu Chen,Yongsheng Bao

As urbanization spreads, more fossil fuels are continuously needed, though they cause air pollution to worsen. The capture and storage of CO 2 has become an area of intense research interest, as it could inhibit further environmental deterioration. Herein, a novel method of synthesizing nitrogen-doped carbon nanosheet adsorbents with highly developed microporosity is proposed. Using biomass chitosan and graphitic carbon nitride (g-C 3 N 4 ) as starting materials not only ensures economically favorable properties but is also makes the adsorbents ecologically friendly. The amount of nitrogen doping agent and varied activation temperatures were found to be capable of precisely controlling the pore structure and nitrogen content in the resulting product. The CO 2 capture capacity of the KOH-activated adsorbent under optimum conditions (a chitosan/graphitic carbon nitride weight ratio of 6 and activation temperature of 750 °C) was determined to be 3.91 mmol/g at 298 K and 1 bar. We also chose three different potassium salt activators to use in place of the strongly caustic KOH. The test results showed that the resulting porous carbon activated by KAc exhibited CO 2 uptakes of 3.54 (298 K) and 5.64 mmol/g (273 K) at 1 bar. This adsorbent also exhibited fast adsorption kinetics , remarkable recyclability , moderately isosteric heats of adsorption and good CO 2 selectivity over N 2 . The present work will provide new inspiration for biomass-based adsorbents for CO 2 capture.

研究领域: 环境科学 · 材料科学 · 化学工程 · 可持续化学
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Journal of Materials Chemistry A · 2024 · IF 10.7

Constructing metallosalen poly(ionic liquid)s to boost photocatalytic CO2 reduction

Xi Chen,Wei Zhou,Xu Fang,Cheng Li,Die Cong,Tie Yu,Wei-Qiao Deng,Chengcheng Liu

Photocatalytic CO2 reduction to syngas has recently garnered substantial interest due to its mild reaction conditions, high safety, and environmental sustainability. However, the efficiency of syngas production remains relatively low. In this study, we have developed metallosalen-based poly(ionic liquid)s (PILs) to enhance syngas production, achieving one of the highest production rates recorded to date. The Co(Salen)-PIL demonstrates a syngas production rate of 168.1 mmol g−1 h−1, including a CO production rate of 69.3 mmol g−1 h−1, which is more than eight times higher than that of the best previously reported organic materials. Mechanistic investigations reveal that pyridine ions facilitate electron transfer from the heptazine light-harvester to the Co(Salen) active site. This study lays the groundwork for developing high-performance catalysts for photocatalytic syngas production.

CAS / MDL: 31175-20-9
研究领域: 材料科学 · 环境科学 · 化学工程
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Journal of CO2 Utilization · 2020 · IF 5.993

Bimetal based inorganic-carbonic anhydrase hybrid hydrogel membrane for CO2 capture

Huan Wen,Lei Zhang,Yingjie Du,Ziyuan Wang,Yunhong Jiang,Hongjie Bian,Jiandong Cui,Shiru Jia

In this study, we synthesized for the first time a bimetal-based inorganic-carbonic anhydrase (CA) hybrid nanoflower to immobilize CA using Cu 2+ and Zn 2+ instead of single metal ion. Subsequently, the synthesized bimetallic hybrid nanoflowers (CANF) were embedded into the poly(vinyl alcohol) (PVA)-chitosan (CS) hydrogel networks to obtain PVA/CS@CANF hydrogel membrane. The CANF exhibited a significantly higher activity recovery of 70 % compared with 35 % with CA/Zn 3 (PO 4 ) 2 hybrid nanoflowers and 10 % with CA/Cu 3 (PO 4 ) 2 hybrid nanoflowers. The PVA/CS@CANF hydrogel membrane possessed excellent mechanical strength, high catalytic activity, and were easy to flow out without centrifugation or filtration. At the same time, the PVA/CS@CANF displayed higher thermostability, storage stability, and pH stability than free CA and CANF , and superior reusability and CO 2 capture capacity. The hydrogel membrane maintained more than 75 % of its original activity after 8 cycles. However, CANF only maintained 12 % of its original activity. Furthermore, the amount of CaCO 3 produced by PVA/CS@CANF membrane was 9.0-fold and 2.0-fold compared with free CA and CANF, respectively. Therefore, This approach to synthesizing bimetallic-based protein hybrid hydrogel membrane could have a bright future in CO 2 capture.

研究领域: 生物化学 · 材料科学 · 环境科学
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LANGMUIR · 2023 · IF 3.9

Porous Polymer Supported Amino Functionalized Ionic Liquid for Effective CO2 Capture

Jianmeng Wu,Zeying Yang,Jiaqi Xie,Peng Zhu,Jiajiao Wei,Renzhe Jin,Hui Yang

A decrease in CO2 emissions is urgently required in the present situation due to the fast growth of carbon dioxide (CO2) in the atmosphere, which has caused a series of global climate issues. This study used an impregnation–evaporation method to immobilize an amino functionalized ionic liquid [C2OHmim][Lys] on a chromatographic column filler GDX-103 and create a novel supported ionic liquid. The results showed that the supported ionic liquid with 60 wt % ionic liquid content had the best adsorption performance at 40 °C, and the CO2 adsorption isotherm showed that the adsorption capacity at 0.1 MPa was 1.29 mmol CO2/g sorbent, which was 6 times greater than the adsorption capacity of the pure carrier. The sample with 60% ionic liquid content has an adsorption capacity of 1.02 mmol CO2/g sorbent under the condition of CO2/N2 mixed gas with 10% CO2 content. This is 43 times greater than the adsorption capacity of the pure carrier, and its adsorption performance is stable after three adsorption and desorption cycles. Through the rich porous structure of GDX-103, the ionic liquid is effectively supported and dispersed, which expands the contact area between CO2 and ionic liquid and enhances the mass transfer of CO2. At the same time, CO2 can be chemically bound to the groups on the anion of ionic liquid and be immobilized, so it has a high selective adsorption capacity of CO2, which makes it a great alternative to traditional CO2 adsorbents.

研究领域: 环境科学 · 化学工程
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JOURNAL OF POROUS MATERIALS · 2023 ·Vol. 30 ·期 6 ·2129-2137 · IF 2.6

Seeds-assisted synthesis of Zr-based metal-organic framework (MIP-202) for efficient adsorption separation of CO2/CH4 and CO2/N2

Tao Ruyu,Liu Hao,Xiang Pan,Lin Yichao,Zhou Junjie,Zhou Chen,Zhao Yayun,Tian Ziqi,Zhang Qiuju

Nanoscale Zr-based metal-organic framework (MIP-202) particles were successfully prepared via a seeds-assisted hydrothermal secondary synthesis. The uniformly-shaped MIP-202 particles exhibit excellent performance on selective CO 2 adsorption from CO 2 /CH 4 and CO 2 /N 2 mixtures. At 298 K and 1 bar, the uptake ratios of CO 2 /CH 4 and CO 2 /N 2 of MIP-202 particles are as high as 32.6 and 65.2, respectively. The IAST (ideal adsorbed solution theory)-predicted selectivities of CO 2 /N 2 (50/50, v/v) and CO 2 /CH 4 (50/50, v/v) reach to 4.5 × 10 10 and 102.2, respectively. The breakthrough experiments further demonstrate that the CO 2 /CH 4 and CO 2 /N 2 mixtures can be efficiently separated through an adsorption column packed with MIP-202 particles. In addition, the as-prepared MIP-202 particles had a low iso-enthalpy of adsorption of CO 2 of 32.95 kJ/mol, which is favorable for the regeneration of the adsorbent. Herein the as-prepared MIP-202 is a potential material for efficient separation of CO 2 from CH 4 or N 2 through an energy- and cost-saving CO 2 capture process.

研究领域: 材料科学 · 环境化学 · 能源工程 · 纳米技术
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Journal of CO2 Utilization · 2019 · IF 5.189

CO2 utilization: Direct power generation by a coupled system that integrates photocatalytic reduction of CO2 with photocatalytic fuel cell

Fengjia Xie,Rong Chen,Xun Zhu,Qiang Liao,Dingding Ye,Biao Zhang,Youxu Yu,Jinwang Li

Carbon dioxide (CO 2 ) as greenhouse gas is the primary cause of global warming. One of the ideal routes to remedy CO 2 emission is to transform it to hydrocarbons by photocatalytic reduction of CO 2 . However, poor yield and product selectivity of photocatalytic reduction of CO 2 pose significant challenges to its widespread applications. To address this critical issue, a coupled system that integrates photocatalytic reduction of CO 2 with photocatalytic fuel cell (PFC) is developed for direct power generation using CO 2 . In this coupled system, the products by photocatalytic reduction of CO 2 works as the fuels for the PFC to directly generate electricity. Direct power generation by this coupled system is demonstrated via only in the presence of CO 2 as the input under illumination. A short circuit current density of 0.175 mA/cm 2 and a maximum power output of 0.110 mW/cm 2 are yielded for the case with the supply of CO 2 , which are much higher than those without CO 2 . Moreover, it is interesting to find that the fuel concentrations at the PFC outlet are even higher than those at the PFC inlet, implying that the coupled system proposed in this study can not only generate the electricity but also yield the solar fuels. This work opens a new avenue for the CO 2 utilization toward direct power generation.

CAS / MDL: 25322-68-3
研究领域: 环境科学 · 能源工程 · 化学工程 · 材料科学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Integration of [Cr3O(HCOO)6(H2O)3]NO3 into MIL-101(Cr) for enhanced separation of CO2/N2 mixture

Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren

Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.

研究领域: 材料科学 · 环境科学 · 化学工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Carbon-embedded Ni catalysts for highly efficient CO2 methanation

Zhihao Liu,Yachao Li,Kangzhou Wang,Yan Li,Yurong He,Jie Liang,Jianli Zhang,Tian-sheng Zhao,Noritatsu Tsubaki,Xinhua Gao

The design and preparation of highly active and stable Ni-based catalysts has attracted extensive attention. In this study, a series of embedded Ni@C catalysts were synthesized by a facile sol-gel method. After reduction at 400 °C, the optimized Ni@C-400 catalyst showed excellent performance in CO 2 methanation at a low temperature of 300 °C, with a CO 2 conversion of 74.3 % and good stability for 70 h. The characterization results indicated that after reduction treatment, the carbon species in the precursor were transformed into graphite carbon with more disorder defects. This structure facilitated the anchoring effect of the nickel components in the Ni@C catalyst, thereby forming a distinctive embedded structure that ensured the preservation of the nickel active phase in the catalyst following prolonged reaction. Therefore, the Ni@C catalyst prevented severe sintering and loss of loaded nickel. In addition, the interaction between Ni and C facilitated charge transfer, enhancing the CO 2 activation.

研究领域: 催化材料 · 化学工程 · 纳米技术
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Nature Communications · 2021 ·Vol. 12 ·期 1 ·1-10 · IF 14.919

Sustained CO2-photoreduction activity and high selectivity over Mn, C-codoped ZnO core-triple shell hollow spheres

Sayed Mahmoud,Xu Feiyan,Kuang Panyong,Low Jingxiang,Wang Shengyao,Zhang Liuyang,Yu Jiaguo

Solar conversion of CO 2 into energy-rich products is one of the sustainable solutions to lessen the global energy shortage and environmental crisis. Pitifully, it is still challenging to attain reliable and affordable CO 2 conversion. Herein, we demonstrate a facile one-pot approach to design core-triple shell Mn, C-codoped ZnO hollow spheres as efficient photocatalysts for CO 2 reduction. The Mn ions, with switchable valence states, function as “ionized cocatalyst” to promote the CO 2 adsorption and light harvesting of the system. Besides, they can capture photogenerated electrons from the conduction band of ZnO and provide the electrons for CO 2 reduction. This process is continuous due to the switchable valence states of Mn ions. Benefiting from such unique features, the prepared photocatalysts demonstrated fairly good CO 2 conversion performance. This work is endeavoured to shed light on the role of ionized cocatalyst towards sustainable energy production.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 环境科学 · 化学工程 · 能源科学
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