Energy & Environmental Science
·
2019
·Vol. 12
·期 8
·2455-2462
·
IF 33.25
Zhenglei Yin,Hanqing Peng,Xing Wei,Huan Zhou,Jun Gong,Mingming Huai,Li Xiao,Gongwei Wang,Juntao Lu,Lin Zhuang
The electrochemical conversion of CO2 to fuels or chemicals is an attractive approach that can combine sustainable energy utilization and carbon recycling, but its practicability is still vague, because the CO2 reduction reaction (CO2RR) has hitherto been mostly studied in electrolyte solutions, with small current densities limited by the solubility of CO2. An important and urgent task is thus to develop CO2 electrolyzers that can demonstrate the feasibility of the large-scale conversion of CO2, in particular analogs of water electrolyzers using polymer electrolyte based gas-diffusion electrodes. Here we report a high-performance CO2 electrolyzer making use of alkaline polymer electrolytes (APEs). A highly conductive and stable APE, quaternary ammonia poly(N-methyl-piperidine-co-p-terphenyl) (QAPPT), was applied both as the membrane separator and the ionomer impregnating the gas-diffusion electrodes. Dry CO2 was fed into the Au cathode, with a faradaic efficiency of CO production (COFE) over 85%, and the oxygen evolution reaction (OER) occurred at the IrO2 anode fed with pure water. The cell was operated at temperatures up to 80 °C, and the current density reached 0.5 A cm−2 at 3 V at 60 °C. The stability of this electrolyzer was tested under 0.1 A cm−2, and the cell voltage remained stable at 2.25 V over 100 h, with the COFE staying at 90–95%.
研究领域:
电化学
·
可再生能源
·
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Wenbo Chen,Zhenguo Zhang,Cancan Yang,Jing Liu,Hongcheng Shen,Kai Yang,Zhe Wang
In this work, we fabricated PIM-based mixed matrix membranes (MMMs) containing MOF-801/ionic liquid nanocomposites to enhance CO 2 separation performance of pure polymer membranes. All membranes and MOF-801/ionic liquid nanocomposites were prepared by solution casting method and wet impregnation, respectively. The samples were analyzed by SEM, XRD , FTIR, TGA and Nitrogen adsorption-desorption measurements. The nanocomposites are composed of metal-organic framework (MOF) MOF-801 and ionic liquid (IL) adsorption capacity. MOF-801 can well control the dispersion of IL in the polymer matrix , which is conducive to exposing more active sites in the nanocomposites to improve the CO 2 adsorption selectivity of MOF-801/ionic liquid nanocomposites. At the same time, the porous structure of nanocomposites also enhances the gas adsorption and diffusion, thereby improving the gas separation performance. Compared with pure PIM-1 membranes, the CO 2 permeability and CO 2 /N 2 selectivity of IL@MOF/PIM-5% MMMs was increased by 129% and 45% (CO 2 = 9420 Barrer, CO 2 /N 2 = 29）, respectively. Compared with MOF-801/PIM-1 MMMs, the permeability of CO 2 decreased slightly but the selectivity of CO 2 /N 2 increased from 27 to 29. The aging test showed that the CO 2 permeability of MMMs could remain above 70% after 90 days. The anti-plasticization performance of MMMs has also been significantly improved. The CO 2 separation performance of IL@MOF/PIM-5% MMMs significantly exceeded the 2008 Robeson upper bound, showing excellent gas separation performance and working stability.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shuang Zheng,Shaojuan Zeng,Guilin Li,Xiaoqian Yao,Zhengchen Li,Xiangping Zhang
Effective capture of trace CO 2 in atmosphere or confined spaces to ensure human beings safety draw a lot of attention, however, how to simultaneously improve CO 2 capacity and selectivity still faces great challenge. Herein, combining porous molecular sieves (SBA-15 and MCM-41) and the anion-functionalized ionic liquid (IL) tetraethylammonium glycinate ([N 2222 ][Gly]), a series of hierarchically porous IL composites with different IL loadings were designed and prepared. Compared with pristine supports, the incorporation of [N 2222 ][Gly] simultaneously improves CO 2 capacity and CO 2 /N 2 selectivity by orders of magnitude, especially for confined spaces (<5000 ppm) and air (415 ppm). When the IL loading was 60 wt%, novel micropores were created, especially ultra-micropores (<0.65 nm), which are not present in bare supports and other [N 2222 ][Gly]@SBA-15 (15, 30 and 45 wt%). Among them, 60 wt%[N 2222 ][Gly]@SBA-15 showed the highest CO 2 uptake of 1.45 and 1.88 mmolCO 2 /g-adsorbent at 0.0005 and 0.005 bar under 313 K along with recyclability, which are much superior to the state-of-the-art reported values. Moreover, superb ideal CO 2 /N 2 selectivity of 11,545 at 0.005 bar and 288 K was achieved, which was 288 times that of SBA-15. Meanwhile, mixed gas breakthrough experiments demonstrated that 60 wt% [N 2222 ][Gly]@SBA-15 shows outstanding CO 2 separation performance under simulative confined spaces and ambient air. The ultra-high CO 2 separation performance was attributed to the synergy of chemical interaction between the IL anion and CO 2 as well as newly created micro- and ultra-micropores effect. This work provides guidelines for the design of IL composites with ultra-micropores for efficient trace CO 2 removal.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Changwei Chen,Yanke Yu,Chi He,Li Wang,Huang Huang,Reem Albilali,Jie Cheng,Zhengping Hao
Four kinds of carbon-based adsorbents (micro-mesoporous hybrid carbon nanosphere and N-doped hollow carbon sphere with single-, double- or ruga-shell morphology) with different structural and textural properties were prepared and systematically studied in CO 2 capture. All synthesized samples possess high specific surface area (828–910 m 2 g −1 ), large pore volume (0.71–1.81 cm 3 g −1 ), and different micropore contents varied from 2.1% to 46.4%. Amongst, the ordered micro-mesoporous carbon nanosphere (OM-CNS) exhibits the best adsorption performance with CO 2 uptake as high as 3.01 mmol g −1 under conditions of 298 K and 1.0 bar, better than most of the reported CO 2 adsorbents. The excellent CO 2 adsorption capacity of OM-CNS can be reasonably attributed to the synergistic effect of ordered mesopore channels and abundant structural micropores which are beneficial for the diffusion and trapping of CO 2 adsorbate. Moreover, the OM-CNS shows excellent CO 2 trapping selectivity and superior stability and recyclability, which endow the OM-CNS as a promising and environmental-friendly adsorbent for CO 2 capture and separation under practical conditions.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yichen Jiang,Dazhi Li,Yifei Zhao,Jianmin Sun
Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH 2 ). The effect of different hydrogen bond donors on CO 2 -epoxide cycloaddition reaction was discussed through XPS, NH 3 -TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO 2 and epichlorohydrin , 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br - , together with the high surface area (1178 m 2 /g), and good CO 2 affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO 2 affinity, excellent catalytic performance in CO 2 cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO 2 capture and conversion.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CORROSION SCIENCE
·
2020
·
IF 6.479
Jixing Wang,Junlei Tang,Hailong Zhang,Yingying Wang,Hu Wang,Bing Lin,Jian Hou,Haibing Zhang
A CO 2 -responsive coating has been developed by adding a thiourea-containing nanocontainer with pH-response release property into an ethyl cellulose coating. The cumulative release of thiourea in the nanocontainer changes with the pH of aqueous solution, which enabled the release rate of thiourea from the nanocontainer in coating to adapt to the change in corrosiveness of 3.5 wt. % NaCl with different dissolved CO 2 content. The results of EIS and immersion experiments showed that this environmental responsive nanocontainer can significantly improve the corrosion resistance of the coating in 3.5 wt. % NaCl solution with and without CO 2 .
研究领域:
材料科学
·
腐蚀工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shujie Liang,Yan Zhang,Jingxian Cong,Jiaxin Lv,Hong Deng
Designing and fabricating nanozymes with photoactivity for CO 2 reduction poses a significant challenge. Here, a hierarchically structured ZFs-tpyNi heterojunction nanozyme, comprising a terpyridine-based Ni complex supported on ZrO 2 nanoframes, has been created through an interfacial engineering strategy for efficient CO 2 reduction under visible light. Due to its unique structural and compositional advantages, ZFs-tpyNi demonstrates superior photocatalytic CO 2 -to-CO conversion compared to its counterpart of ZFs and tpyNi, achieving a CO yield of 18.2 µmol and a selectivity of 92.4 % with a high apparent quantum efficiency of 0.96 % in 3 h. These innovative catalysts also show excellent durability for at least eight cycles without a loss in performance, maintaining a remarkable structural stability with no obvious collapse of its framework and morphology. Systematic investigations reveal that ZFs-tpyNi heterostructures exhibit a high specific surface area advantageous for the effective loading of tpyNi and exposure of active sites. The robust ZFs framework, characterized by extensive porosity, prevents nanoparticle agglomeration and accelerates mass transfer during catalysis. Additionally, the spatially heterogeneous interface enables precise modulation of band alignment and bandgap dynamics in nanozymes, enhancing light absorption and promoting the generation and separation of photogenerated charge carriers. Consequently, the nanozyme demonstrates enhanced CO 2 adsorption and activation capabilities, leading to improved selectivity of catalytic products. This work aims at highlight the role of nanozyme catalysts in sustainable energy production.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 51
·33069-33078
·
IF 4.036
Xia Wang,Wulan Zeng,Chunling Xin,Xiangjun Kong,Xiude Hu,Qingjie Guo
The accumulation and incineration of crop waste pollutes the environment and releases a large amount of CO2. In this study, corncob crop waste was directly activated using solid KOH in an inert atmosphere to prepare porous activated carbon (AC) to capture CO2, and to introduce N-containing functional groups that favour CO2 adsorption, urea was mixed with corncob and KOH to prepare N-doped AC. The physical and chemical properties of the AC were characterized, and the effects of the mass ratio of KOH and urea to corncob, the activation temperature and time as well as regeneration were investigated to explore the optimal preparation process. The pores in the AC are mainly micropores, with the specific surface area and pore volume reaching 926.07 m2 g−1 and 0.40 cm3 g−1 for KOH-activated corncob and 1096.70 m2 g−1 and 0.48 cm3 g−1 after N-doping; the C–O plus O–H ratio and the –NH– ratio, which favour CO2 adsorption in N-doped AC were 6.04 and 1.92%, respectively. The maximum adsorption capacities for KOH-activated corncob before and after N-doping were 3.49 and 4.58 mmol g−1, respectively, at 20 °C and remained at 3.44 and 4.52 mmol g−1 after ten regenerations. The prepared corncob-based AC showed good application prospects for CO2 capture.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Greenhouse Gases-Science and Technology
·
2019
·Vol. 9
·期 3
·553-566
·
IF 1.693
Menglong Liu,Siyang Tang,Kui Ma,Changjun Liu,Hairong Yue,Bin Liang
Monoethanolamine (MEA) solution has been used widely in the post-combustion CO 2 capture process; however, the high heat duty and reaction temperature (e.g. 125°C) for MEA regeneration leads to a high energy requirement (nearly 70–80% of the total running cost). We report the use of solid particles (H-Zeolite Socony Mobile-5 (HZSM-5), quartz, and activated carbon) to facilitate the mass transfer of CO 2 bubble nucleation and enhance the CO 2 desorption rate. The results show that the mass transfer of CO 2 from liquid phase to gas phase is the rate-determining step, rather than the chemical reaction. The addition of HZSM-5 particles in the solution significantly enhanced CO 2 bubble nucleation by providing nucleation sites and gas cavities, leading to an average CO 2 desorption rate enhancement of 43.2%, and an energy consumption reduction of 23.3%. This process also operated at ∼95°C, which is a much lower temperature than that used in the commercial process and is feasible for industrial applications. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Nan Li,Penny Xiao,Weijie Liu,Liying Liu,Zijian Wang,Jian Wang,Peng Gao,Qi Wu,Xinchao Ma,Gang Kevin Li
Compared with traditional commercial adsorbent zeolite pellets, binder-free molecular sieves can provide better adsorption performance. In this paper, we reported a novel method to synthesize binder-free zeolite X pellets (BF-Z), that is, zeolite X powder was intricately combined with halloysite nanotubes (HNTs) using hydroxypropyl methylcellulose (HPMC), and then the sample was calcinated to form crystals, where HPMC was decomposed and HNTs was also completely converted into binder-free X zeolite. The synthesized BF-Z showed the highest CO 2 adsorption capacity of 4.98 mmol/g at 303 K and 1 bar, compared with commercial NaX zeolites produced by Jianlong, Sigma and UOP companies. Calculated by IAST model, the separation coefficient of CO 2 to N 2 (CO 2 /N 2 = 25/75) on BF-Z is 74 at 303 K and 1 bar. The great separation performance of CO 2 from N 2 (CO 2 /N 2 = 25/75) was also exhibited in breakthrough experiments and a designed VSA process. Compared with commercial NaX (UOP), in breakthrough experiment, BF-Z presented high CO 2 adsorption capacity and rapid adsorption rate; and in designed thirty six-step vacuum swing adsorption process (VSA), the six-bed VSA system using BF-Z as adsorbents demonstrated excellent separation performance such as high CO 2 purity and recovery, low energy consumption and enhanced CO 2 production capacity. The notable efficacy of BF-Z in CO 2 adsorption and separation underscores its promising utility in both commercial and industrial settings.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Xinjie Luo,Pengfei Zheng,Ke Gao,Bing Wei,Yujun Feng
Water-alternating-CO 2 gas (WAG) flooding is a common technique to enhance oil recovery via improving CO 2 sweep efficiency, but serious gas channeling may still occur, especially in reservoirs with strong heterogeneity, due to a poor blocking capacity of aqueous slugs to the “channeling” pathway induced by their low viscosity. Herein, a copolymer whose aqueous solution viscosity can be increased by both heat and CO 2 was developed and added into the aqueous slug to control gas channeling and increase oil recovery during enhanced WAG processes. The copolymer was synthesized by grafting poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) onto the triblock copolymer, Pluronic F127, PEO 100 -PPO 65 -PEO 100 . The aqueous copolymer solutions can be thickened/gelled by heating due to the formation of micelles as the physical cross-link and their entanglements even at a concentration as low as 0.2 wt%, and viscosified by bubbling CO 2 thanks to expanded copolymer coils caused by electrostatic repulsion-induced chain extension of protonated PDMAEMA chains. Notably, thermo- and CO 2 -triggered viscosifying can work synergistically and they are completely reversible upon cyclically heating/cooling the copolymer solutions and bubbling/removing CO 2 into/from the aqueous phase, respectively. In WAG flooding tests using two parallel cores, gas channeling was mitigated by blocking high-permeability cores due to in-situ thermo-induced gelation and CO 2 -triggered thickening of copolymer slugs, thus diverting chase fluids into unswept low-permeability cores and enhancing 21–22% total oil recovery than the conventional and HAPM-enhanced WAG modes. Importantly, owing to the characteristics of low initial viscosity, single component, and thermo-gelation, this dually-responsive copolymer possesses high injectivity and satisfactory gelation control. This work could enlighten the design of novel dual/multiple stimuli-thickening polymers used for channeling control and enhanced oil recovery.
研究领域:
石油工程
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Yutong Shen,Jun Xiao,Qijing Wu,Jingting Su,Li Zhu
To improve the conversion efficiency and reduce the CO 2 emissions associated with the reforming of biomass tar to syngas, photothermal catalysts were prepared in this study through various impregnation methods. Photothermocatalytic CO 2 reforming (PTCR) of benzene as a tar model compound, was conducted using the prepared Ni/TiO 2 -Al 2 O 3 catalysts. The results show that the introduction of TiO 2 facilitates the conversion of NiO to Ni during the photothermal reaction, while the photocatalysis of TiO 2 significantly enhances the photothermocatalytic activity of the Ni/Al 2 O 3 catalysts at low temperatures. Moreover, the methodology for catalyst preparation involving the loading of NiO before TiO 2 is also beneficial to catalyst performance. However, when the mass ratio of TiO 2 to Al 2 O 3 exceeds 1, the specific surface area, pore volume, and structural stability of the catalysts are reduced. The results of PTCR experiment show the following optimal Ni/TiO 2 -Al 2 O 3 catalyst preparation parameters: 25% NiO content and a TiO 2 /Al 2 O 3 ratio of 3:7; 450 °C calcination temperature and a nitrogen atmosphere. The maximum benzene conversion achieved through PTCR with the 0.25Ni/0.3Ti0.7Al(M2) catalyst is 88.2%. However, a large amount of coke is deposited onto the spent catalyst surface, contributing significantly to catalyst deactivation.
研究领域:
能源化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）