Sustainable Chemistry for Climate Action
·
2023
·
IF 0
Ya-Qi Ba,Yong-Sheng Wang,Tian-Yi Li,Zhe Zheng,Guang-Ping Hao,An-Hui Lu
CO 2 capture from flue gas is one of the global urgent tasks. Adsorption separation of CO 2 is an energy-efficient way as compared to the absorption method. The central issue is to devise efficient adsorbents that work well under flue gas conditions with temperatures of 323–348 K and low CO 2 concentrations of 15%. In this work, we targeted this issue and proposed a well-controlled diffusion strategy, which is achieved over a series of poly(furfuryl alcohol)-derived carbons (PFCs) with dense and abundant ultra-micropores. As the adsorption temperature increased from 298 to 348 K, the CO 2 capture capacity is 54% kept for PFC-800, which is 1.2 times higher than that for samples without diffusion limitation. The capture of CO 2 is kinetics control at ambient temperature, however, at 348 K CO 2 with higher kinetic energy can overcome the restriction of the narrow pore entrance and the CO 2 /N 2 selectivity for simulated flue gas composition increases from 20 to 40. Furthermore, the PFCs exhibit a high CO 2 volumetric adsorption capacity of 97 cm 3 cm −3 at 298 K and 1 bar, benefiting the practical application deployed with an integrated adsorption column. The diffusion kinetics can be further tuned when altering the bulk phase into nanocoating, which would inspire their application in different scenarios.
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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DOI
AICHE JOURNAL
·
2023
·Vol. 69
·期 6
·e18046
·
IF 3.7
Zhiwei Zhao,Yueyue Liu,Xing Liu,Yuan Liu,Jingwen Chen,Shixia Chen,Shuguang Deng,Jun Wang
The one-step adsorptive separation of high-purity ethylene (C 2 H 4 ) from a ternary gas mixture (C 2 H 2 /C 2 H 4 /CO 2 ) is challenging and has not been reported on porous carbons. Herein, we report camphor seeds husk-derived ultramicroporous carbons (CSHs) show high affinities toward acetylene (C 2 H 2 ) and carbon dioxide (CO 2 ) over C 2 H 4 . The optimized CSH-2-700 with high heteroatom contents and centered pore size distributions shows high C 2 H 2 adsorption capacity (2.24 mmol g −1 ) and record ideal adsorbed solution theory (IAST) C 2 H 2 /C 2 H 4 selectivity (10.2) among one-step C 2 H 4 purification adsorbents. Meanwhile, CSH carbons are the only carbon adsorbents that preferentially adsorb CO 2 over C 2 H 4 , with a CO 2 /C 2 H 4 selectivity of 1.9 under ambient conditions. Furthermore, dynamic breakthrough experiments verified its feasibility for one-step C 2 H 4 purification from a three-component C 2 H 2 /C 2 H 4 /CO 2 gas-mixture.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2015
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IF 6.723
Guojian Chen,Xiaochen Wang,Jing Li,Wei Hou,Yu Zhou,Jun Wang
A family of nitrogen-enriched ultramicroporous carbon materials was prepared by direct carbonization of task-specifically designed molecular carbon precursors of cyanopyridinium-based crystalline dicationic salts (CISs). Varying the molecular structure of CISs, large surface area (918 m2 g–1), high N content (20.10 wt %), and narrow distributed ultramicropores (0.59 nm) can be simultaneously achieved on the sample PCN-14 derived from methyl-linked 4-cyanopyridinium D[4-CNPyMe]Tf2N. It therefore exhibited exceptional performance in greenhouse gas CO2 capture, i.e., simultaneously possessing (1) high CO2 adsorption uptakes: 5.33 mmol g–1 at 273 K, and 3.68 mmol g–1 at 298 K (both at 1.0 bar); (2) unprecedented selectivity of CO2 versus N2: 156; and (3) a high adsorption ratio of CO2 to N2: 148 (at 1.0 bar). This is the first time such a high selectivity and adsorption ratio over carbon materials has been achieved, which is among the highest values over solid adsorbents.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chujie Zhang,Yugao Wang,Jiaxin Jing,Jinping Li,Jiangfeng Yang
Coal-based porous carbon usually has broad pore size distribution, and it remains a major challenge for achieving controllable and optimized pore size distributions in the ultramicroporous (<0.7 nm) range. In this work, coal-derived humic acid-based carbons (HACs) were successfully synthesized by in-situ ionic activation, which consumed much less KOH than the traditional KOH activation method, demonstrating environmentally friendly advantages. The prepared HACs were characterized of the concentrated ultramicroporous pore size distribution. Importantly, ultramicroporous pore size of HACs could be controlled at the sub-angstrom level by slightly adjusting the KOH amount. Dynamic breakthrough experiments and PSA process simulations strongly demonstrated the superior and applicable separation performance of HACs for CH 4 /N 2 mixtures. The investigation extends the application of in-situ ionic activation in coal-based materials and provides a cheap, green, and efficient coal-based adsorbent for low-concentration coalbed methane enrichment.
研究领域:
材料科学
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环境科学
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能源工程
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Chengyao Zhao,Yiming Lin,Qiaoyan Lin,Qi Liu,Yujing Liu,Zhongqiu Liu,Anguo Ying
Aqueous zinc-ion hybrid capacitors (ZIHCs) are a promising new type of energy storage device, but there is a plight that the unsatisfactory Zn 2+ storage capability of carbonaceous cathodes limits further application. To address this issue, desolvation strategy is employed to tailor the solvation sheath of Zn 2+ in the ultra-micropores (0.59 nm) nanospheres , where H 3 PO 4 acts as phosphorus source for forming C-P bonds and enhancing C=O bonds to further reduce the desolvation energy barrier. In practical application, a quasi-solid-state flexible ZIHC is constructed, which provides a battery-level energy density (293.4 Wh kg −1 ) at a power density (180 W kg − 1 ) and a remarkable capacity retention of 93.4 % after 10 000 cycles. Electrochemical analyses, DFT calculations and structural characterization reveal that ultra-microporous is proved to be a prerequisite for C-P/C=O that are expected to further deplete solvent molecules within a Zn 2+ solvation sheath. Also, the coupling effect between the strong adsorption of Zn 2+ by C-P/C=O and the hydrophobic effect of C-P play an important role in facilitating desolvation process. This work creates a precedent for the application of ultra-microporous carbon materials in ZHICs and provides a brand-new approach for breaking the bottleneck of the low energy density and poor lifespan of ZHICs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Yajun Wei,Tan Zhao,Jiawei Wang,Yanli Chen,Qiang Wang,Xizheng Liu,Yunfeng Zhao
The development of an ultramicroporous (<7 Å) adsorbent with a narrow pore distribution for capturing and adsorbing gas molecules has received a lot of attention. In this paper, the commercial carbon molecular sieve (CMS) was used as the precursor, and a carbon molecular sieve (CMS-A-5) with better performance was obtained by activating with potassium hydroxide (KOH). After activation, the ultramicroporous volume increased from 0.163 cm3 g–1 (CMS) to 0.329 cm3 g–1 (CMS-A-5), and the CO2 capacity increased from 42.76 to 71.92 cm3 g–1 at 298 K and 1 bar. The breakthrough experiments demonstrated that the CO2 capture ability of CMS-A-5 increased by ∼9.5 times for the respiratory air containing CO2/O2/N2 (4:20:76) and was easily regenerated and reused. CMS-A-5 was also capable of selectively capturing VOC molecules including benzene, toluene, and C8 alkyl aromatics (BTEX) with a high adsorption capacity at a low pressure. The excellent CO2 and VOC molecule adsorption capacity make CMS-A-5 a promising candidate for selective separation of the gas mixture, in particular, for air purification in confined spaces.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
AICHE JOURNAL
·
2021
·Vol. 67
·期 9
·e17281
·
IF 3.993
Ze Dong,Bei Li,Hua Shang,Peixin Zhang,Shixia Chen,Jiangfeng Yang,Zheling Zeng,Jun Wang,Shuguang Deng
The adsorptive separation of CH 4 from low-grade coal-bed gas can be performed at decentralized and remote coal mines, and it uses more energy- and is cost-efficient than the traditional cryogenic distillation process. Herein, we present a facile method to prepare ultramicroporous carbon granules with a narrow pore-size distribution at 0.5–0.6 nm. To our knowledge, such centered and uniform pore-size distribution in carbon granules has never been reported. The carbon granules can be directly utilized in adsorption columns without a granulation or pelletization process. The granular oil-tea-shell-derived porous carbon (GOC-2) exhibited a record-high CH 4 uptake of 1.82 mmol/g and CH 4 /N 2 selectivity of 5.8 at 1.0 bar and 298 K among carbon granules. The excellent CH 4 /N 2 separation performances were confirmed from the results of dynamic breakthrough experiments and pressure swing adsorption simulations. This work provides a novel strategy for developing ultramicroporous carbon granules and guides the future design of efficient CH 4 /N 2 separation adsorbents.
研究领域:
材料科学
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能源工程
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DOI
高影响因子
ACS Materials Au
·
2025
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IF 6.5
Man Liu,Weiwei Shi,Huili Liu,Yanzhen Guo,Baocheng Yang,Binbin Chang
Carbon capture has emerged as a pivotal carbon neutrality technology for addressing greenhouse effect challenges. Porous carbons are one of the most promising adsorbents for CO2 capture and separation from flue gas, yet their traditional synthesis necessitates inert atmospheres to avoid oxidation, which greatly restricts the large-scale production at a low cost and advanced industrial applications. Herein, we propose an innovative pathway for large-scale fabrication of porous carbons via one-step pyrolysis in an air environment. Porosity and surface chemistry can be concurrently tailored by controlling the air-assisted pyrolysis process, and the optimization mechanism is unveiled in detail. The resultant materials feature well-interconnected hierarchical porosity with highly proportioned ultramicroporosity, uniform spherical morphology, and high surface heteroatom doping levels. By leveraging porosity and surface chemistry, the optimal sample exhibits superior CO2 capture behaviors of satisfactory CO2 uptake and ultrahigh selectivity. CO2/N2 selectivity reaches up to 160 at 0.15 bar and 25 °C, and it still achieves up to 76 at 1.0 bar and 25 °C, ranking it in the top 5% of the reported porous carbons. We explore the correlations between porosity, surface heteroatoms, and CO2 capture behaviors. Porosity has a decisive function on CO2 capture capacity and selectivity, especially ultramicroporosity, and surface heteroatoms doping could have a positive promotion in selectivity caused by extra CO2-philic sites. This work pioneers a feasible approach for large-scale directional design of functional porous carbons through air-assisted pyrolysis under mild conditions.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Nano-Micro Letters
·
2020
·Vol. 12
·期 1
·1-17
·
IF 12.264
Ding Chenfeng,Liu Tianyi,Yan Xiaodong,Huang Lingbo,Ryu Seungkon,Lan Jinle,Yu Yunhua,Zhong Wei-Hong,Yang Xiaoping
An ultra-microporous carbon material simultaneously with high specific surface area (1554 m 2 g −1 ) and packing density (1.18 g cm −3 ) is designed and fabricated.
The resulting carbon material integrates the high gravimetric and volumetric capacitance (430 F g −1 and 507 F cm −3 at 0.5 A g −1 ) and thereof provides the robust all-solid-state cellulose supercapacitor with high areal and volumetric density.
研究领域:
材料科学
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能源存储技术
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产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 13
·3208-3219
·
IF 6.813
Wei Hui,Xin-Yi Xu,Fei-Feng Mao,Ling Shi,Hai-Jun Wang
Porous carbon materials have shown great promise for the efficient capture and conversion of atmospheric CO2, but remain challenging. In this work, activated N/O-rich multilayer ultramicroporous carbon materials for the effective capture and conversion of atmospheric CO2 have been generated using a simple one-step method. Notably, the developed catalyst has a multilayered ultramicroporous framework and double N/O heteroatoms as active sites, which capture and activate atmospheric CO2 for the cycloaddition reaction simultaneously, obtaining 96% yield of cyclic carbonate. Additionally, the stable recyclability of the catalyst highlights the sustainability of the efficient conversion of CO2 to cyclic carbonates under mild conditions. Meanwhile, the low isosteric heat of CO2 adsorption is measured to be around 14.8–19.1 kJ mol−1, which means that the energy consumption of the CO2 desorption process would be quite low in industrial application. We believe that this work has tremendous potential for industrial CO2 capture and conversion into high-value-added products.
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
Nano Energy
·
2017
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IF 12.343
Qizhen Zhu,Qian Zhao,Yabin An,Babak Anasori,Haoran Wang,Bin Xu
Lithium-sulfur (Li-S) batteries are one of the most promising energy storage systems with high energy density . However, they suffer from fast capacity fading due to the shuttle of the dissolved polysulfides . Using small sulfur molecules (S 2–4 ) as cathodes can avoid the shuttle problem, but the preparation of ultra-microporous carbon to encapsulate S 2–4 is challenging. Here, we report a Li-S battery with an excellent cycling performance by using a unique ultra-microporous carbon (UMC) with a uniform pore size of 0.55 nm. The UMC was synthesized from PVDF via a facile pyrolysis process to only accommodate small S 2–4 molecules and eliminate large S 8 molecules. This S/UMC composite electrode is compatible with the carbonate-based electrolyte used in Li-S batteries. The resulting battery shows a typical discharging profile with only one long potential plateau because the reductions from cyclo-S 8 to dissolved polysulfides and consequence shuttle problem are avoided. The S/UMC composite retains a capacity of about 852 mAh g −1 and Coulombic efficiency approaching 100% after 150 cycles at 0.1 C and delivers a long-term cycling at 1 C for 1000 cycles with only around 0.03% capacity loss per cycle. We also tested this S/UMC composite electrode in Na-S systems and observed similar electrochemical behaviour. These results indicate that the S/UMC composite is a promising candidate as an electrode material in Li-S and Na-S batteries and related systems.
研究领域:
材料科学
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电化学
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能源存储
·
纳米材料
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电池技术
✓ 已验证
DOI
高影响因子
DESALINATION
·
2025
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IF 9.8
Lirong Bi,Xinwei Sui,Shuo Tian,Xiaowei Liu,Shicheng Ma,Zhongqiu Liu,Yujing Liu,Anguo Ying
Flow electrode capacitive deionization (FCDI) holds great promise for next-generation desalination, yet its advancement is fundamentally constrained by sluggish electron conduction and poor ion selectivity under multivalent interference. Herein, we conceive a semi-anchoring strategy that covalently binds polymeric ionic liquids (PILs) onto ultra-microporous carbon nanospheres (UCNs), constructing a UCNs@PILs composite featuring an ion-selective charge percolation network. This design unlocks dual-functionality: it not only enhances electron mobility via continuous conductive pathways, but also enables sodium-preferred transport through a synergistic “push-pull” effect, as revealed by DFT and COMSOL simulations. Strikingly, this strategy allows the carbon slurry loading to be reduced from the conventional 5-15 wt% [1] to just 3.33 wt% without conductive additives, approaching the lowest value ever reported in FCDI. As a result, the system delivers a 28.00 % increase in desalination efficiency, an 18.26 % reduction in energy consumption, and a 39.40 % enhancement in ion selectivity, while its ion selectivity matches that of state-of-the-art carbon-based materials. This work not only overcomes electron conduction discontinuity and ion transport limitations, but also establishes the semi-anchoring framework for achieving ultra-low percolation thresholds with high ion selectivity, offering a new paradigm for the scalable design of advanced FCDI electrodes.
研究领域:
环境科学
·
材料科学
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化学工程
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能源技术
·
水处理技术
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产品关联
DOI
高影响因子