Green Energy & Environment
·
2020
·
IF 6.395
Li Ma,Yu Qiu,Min Li,Dongxu Cui,Shuai Zhang,Dewang Zeng,Rui Xiao
The chemical looping process, where an oxygen carrier is reduced and oxidized in a cyclic manner, offers a promising option for hydrogen production through splitting water because of the much higher water splitting efficiency than solar electrocatalytic and photocatalytic process. A typical oxygen carrier has to comprise a significant amount of inert support, to maintain stability in multiple redox cycles, thereby resulting in a trade-off between the reaction reactivity and stability. Herein, we proposed the use of ion-conductive yttria-stabilized zirconia (YSZ) support Fe 2 O 3 to prepare oxygen carriers materials. The obtained Fe 2 O 3 /YSZ composites showed high reactivity and stability. Particularly, Fe 2 O 3 /YSZ-20 (oxygen storage capacity, 24.13%) exhibited high hydrogen yield of ∼10.30 mmol g −1 and hydrogen production rate of ∼0.66 mmol g −1 min −1 which was twice as high as that of Fe 2 O 3 /Al 2 O 3 . Further, the transient pulse test indicated that active oxygen diffusion was the rate-limiting step during the redox process. The electrochemical impedance spectroscopy (EIS) measurement revealed that the YSZ support addition facilitated oxygen diffusion of materials, which contributed to the improved hydrogen production performance. The support effect obtained in this work provides a potentially efficient route for the modification of oxygen carrier materials.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Zhong Ma,Chuan Yuan,Shuai Zhang,Yonggang Lu,Junhui Xiong
Chemical looping combustion (CLC) is a clean and efficient flame-free combustion technology, which combust the fuels by lattice oxygen from a solid oxygen carrier with inherent CO 2 capture. The development of oxygen carriers with low cost and high redox performance is crucial to the whole efficiency of CLC process. As the solid by-product from the sulfuric acid production, pyrite cinder presented excellent redox performance as an oxygen carrier in CLC process. The main components in pyrite cinder are Fe 2 O 3 , CaSO 4 , Al 2 O 3 and SiO 2 in which Fe 2 O 3 is the active component to provide lattice oxygen. In order to systematic investigate the functions of supports (CaSO 4 , Al 2 O 3 and SiO 2 ) in pyrite cinder, three oxygen carriers (Fe 2 O 3 -CaSO 4 , Fe 2 O 3 -Al 2 O 3 and Fe 2 O 3 -SiO 2 ) were prepared and evaluated in this study. The results showed that Fe 2 O 3 -CaSO 4 displayed high redox activity and cycling stability in the multiple redox cycles. However, both Fe 2 O 3 -Al 2 O 3 and Fe 2 O 3 -SiO 2 experienced serious deactivation during redox reactions. It indicated that the inert Fe-Si solid solution (Fe 2 SiO 4 ) was formed in the spent Fe 2 O 3 -SiO 2 sample, which decreased the oxygen carrying capacity of this sample. The XPS results showed that the oxygen species on the surface of Fe 2 O 3 -CaSO 4 could be fully recovered after the 20 redox cycles. It can be concluded that CaSO 4 is the key to the high redox activity and cycling stability of pyrite cinder.
研究领域:
能源科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2014
·
IF 0
Delong Ma,Zhong Wu,Zhanyi Cao
Supercapacitors (SCs) have attracted much attention as one of the alternative energy devices due to their high power performance, long cycle life, and low maintenance cost. Graphene is considered as an innovative and promising material due to its large theoretical specific surface area, high electrical conductivity , good mechanical properties and chemical stability. Herein, we report an effective strategy for elaborately constructing rationally functionalized self-standing graphene (SG) obtained from giant graphene oxide (GGO) paper followed by an ultrarapid thermal-processing. This treatment results in both the exfoliation of graphene sheets and the reduction of GGO by elimination of oxygen-containing groups. The as-prepared SG electrode materials without additive and conducting agent provide an excellent combination of the electrical double layer capacitor (EDLC) and pseudocapacitor (PC) functions and exhibit superior electrochemical performance, including high specific capacitance, good rate capability and excellent cycling stability when investigated in three-electrode electrochemical cells .
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
Applied Water Science
·
2022
·Vol. 12
·期 11
·1-9
·
IF 5.411
Chen Gangling,Zhang Jianying,Geng Miaomiao,Sunarso Jaka,Wong Ngie Hing,Ma Tianlin,Wang Yujie,Chen Guihua
The support for the membrane is the basis for the preparation and application of the zeolite membrane. Moreover, its cost and properties directly determine the performance of the zeolite membrane and its industrial applications. A novel porous silicon carbide (SiC) support for zeolite membrane bonded with needle-like mullite (3Al 2 O 3 ·2SiO 2 ) was prepared using SiC powders as the raw material and kaolin, Al(OH) 3 , and AlF 3 as the needle-like mullite precursor additives via an in situ high-temperature reactions in an air atmosphere. Effects of the support material composition and the sintering temperature on the sintering behavior, pore structure, permeability, and microstructure of the resultant supports were extensively investigated. The needle-like mullite formation consumed silicon oxide (SiO 2 ) and generated a rigid skeleton structure with a good pore structure and bonding phase. Hence, the porous SiC support exhibited high porosity, with relatively large pore size and mechanical strength, which helped improve the support performance. Notably, the porous SiC support sintered at 1480 °C with in situ inter-particle needle-like mullite bonding exhibited excellent filtration and permeability performance. The porous support materials and methods used in this work are suitable for designing and preparing a novel porous SiC support for zeolite membranes.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 17
·25273-25286
·
IF 0
Chen Junxia,Yang Zhenzhen,Li Weigang,Yang Yuying,Zhu Feng,Huo Zongli,Zhou Qing
The poor conductivity, poor stability, and agglomeration of iron-based metal organic framework MIL-88A(Fe) limit its application as persulfate (PS) activator in water purification. Herein, MXene-supported MIL-88A(Fe) composites (M88A/MX) were synthesized to enhance its adsorption and catalytic capability for tetracycline (TC) removal. Scanning electron microscope (SEM), X-ray diffractometer (XRD), Fourier transform infrared spectrometer (FT-IR), and X-ray photoelectron spectroscopy (XPS) were used to characterize prepared materials, confirming the successful attachment of MIL-88A(Fe) to the surface of MXene. M88A/MX-0.2 composites, prepared with 0.2 g MXene addition, exhibit optimal degradation efficiency, reaching 98% under conditions of 0.2 g/L M88A/MX-0.2, 1.0 mM PS, 20 ppm TC, and pH 5. The degradation rate constants of M88A/MX-0.2 were 0.03217 min −1 , which was much higher than that of MIL-88A(Fe) (0.00159 min −1 ) and MXene (0.00626 min −1 ). The removal effects of reaction parameters, such as dosage of M88A/MX-0.2 and PS; initial solution pH; and the presence of the common co-existing constituents (humic acid and the inorganic anions) were investigated in detail. Additionally, the reuse of M88A/MX-0.2 showed that the composites had good cycling stability by recurrent experiments. The results of electron paramagnetic resonance (EPR) and quenching experiments indicated that ·OH, ·SO 4 − , and ·O 2 − were involved in the M88A/MX-0.2/PS system where persulfate oxidation process was activated with prepared M88A/MX-0.2. In addition, the intermediates of photocatalytic degradation were determined by HPLC–MS, and the possible degradation pathways of the target molecules were inferred. This study offered a new avenue for sulfate-based degradation of Fe-based metal organic framework.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
PubMed
NANOTECHNOLOGY
·
2018
·Vol. 29
·期 42
·425708
·
IF 3.404
Hongjun You,Yingying Xuan,Yun Zuo,Fei Shen,Xiaogang Han,Jixiang Fang
An ideal supporting material improves both activity and durability of noble metal nanoparticles in electrocatalytic reactions. Graphene possesses a high transport rate of electrons in-plane, a low cost, and stability, but, the restacking of graphene layers trap noble metal nanoparticles and make them inaccessible to reactants and results in reduced catalytic activity. Here, holey-graphene as the supporting materials for Pt nanoparticle catalysts is deeply investigated in the electrocatalytic reaction of methanol oxidation. The holey-graphene can be scalable to synthesize using our simple method described herein. The holes on the holey-graphene layer promote the access of reactants with Pt nanoparticle catalysts compared with carbon black and graphene when used as supporting materials. Density functional theory calculations and molecule dynamic simulation further explain the function of holey-graphene in the promotion of electrocatalytic activity. Holey-graphene may open extraordinary possibilities as a supporting material for electrocatalysts.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Royal Society Open Science
·
2020
·Vol. 7
·期 8
·
IF 2.646
Jiawei Chen,Fangfang Liu,Yongfeng Li,Yongshen Dou,Sanmao Liu,Liangjun Xiao
The zeolite monoliths were synthesized by a facile polymer scaffold template assisted hydrothermal method. The selected foam-shaped template of a polyurethane (PU) foam monolith, was used to prepare the self-standing zeolite foam (ZF) monolithic materials. The obtained ZF products can preserve the same size, shape and macroporous network structure of the original PU foam scaffold template, although the zeolite nano-crystallites had been fully substituted for the PU template to form the new skeleton struts and walls. The as-synthesized ZF products demonstrated abundant hierarchical porosity (involving triple micro-, meso- and macropores). Meanwhile, compared with the conventional zeolite powders, the self-standing ZF monolithic materials exhibited greater total pore volume and nearly three times higher mesopore volume, suggesting wider applications as catalysts, catalyst supports and adsorbents in industry.
研究领域:
材料科学
·
化学工程
·
催化材料
✓ 已验证
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Heyu Li,Minghua Liu,Wenqi Zou,Yuancai Lv,Yifan Liu,Lihui Chen
In this study, Ni-metal–organic frameworks (MOFs) were used as precursors to obtain carbon-supported nickel composites (Ni@C) after calcination. The hydrodeoxygenation properties of the model compound and corncob lignin were investigated without an external hydrogenation source and initial pressure. Additionally, the effect of Ni@C on degradation of model compounds, corncob lignin, and benzyl phenyl ether (BPE) under different conditions was examined. The results showed that with isopropanol as the in situ hydrogen source, the conversion percentage of BPE was 90.2% and the yield of phenol was 88.3 wt % at 150 °C. The catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), NH3 temperature-programmed desorption (NH3-TPD), X-ray photoelectron spectroscopy (XPS), and thermogravimetry (TG), and the lignin and bio-oil were characterized by gas chromatography–mass spectrometry (GC–MS) and two-dimensional heteronuclear single quantum coherence (2D-HSQC). It was found that the Ni@C catalyst with well dispersion, high support rate, and rich acid sites was successfully synthesized. In the process of degradation, the C–O ether bond in the structure of lignin was successfully broken to generate the phenolic monomer, and the high-efficiency hydrodeoxygenation of lignin was realized under mild conditions.
研究领域:
化学工程
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生物质能
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2016
·
IF 3.611
Yingchao Hu,Wenqiang Liu,Hongqiang Chen,Zijian Zhou,Wenyu Wang,Jian Sun,Xinwei Yang,Xian Li,Minghou Xu
A screening of inert solid supports as metal skeletons of CaO-based sorbents was conducted in this work, aiming to provide the basis and guideline for the selection of inert solid refractories to produce high temperature CO 2 capture sorbent. We studied 12 different refractories including Al-, Ti-, Mn-, Mg-, Y-, Si-, La-, Zr-, Ce-, Nd-, Pr- and Yb-based supports, among which Yb and Pr are newly introduced ones. The sorbents were synthesized using the same wet-mixing method, by which the inert supports could be well dispersed among the ultra-fine active specie of CaO/CaCO 3 particles to fully play the role of frameworks for sintering resistance. The sorbents stabilized by these inert supports were also cyclically tested under the same conditions. Y- and Al-based supports were found to exhibit much superior cyclic performance than the other supports. Mn-, Mg-, La-, Yb- and Nd-based supports are also good candidates, whereas the other ones containing Ti-, Ce-, Zr-, Si- and Pr-based supports show less effectiveness. The melting point of the inert support and surface area of the synthetic sorbents are found to be the key factors to affect the sorbent performance.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Wangwu Li,Jiao Peng,Hui Li,Zhenyu Wu,Yuehua Huang,Baobao Chang,Xiaowei Guo,Gairong Chen,Xianyou Wang
At present, the main limitations for the practical application of silicon (Si) as an anode material of a lithium-ion battery are huge volume variation and low electrical conductivity. Core–shell silicon/carbon (Si/C) composites can greatly relieve the Si large volume change and accelerate the low Li+ conductivity; however, cracking of carbon shell and the failure of the electrode structure still limit the lithium storage capability and cyclic life. Herein, a flexible freestanding N-doped core–shell Si/C nanofiber (SC-NF) anode is prepared by the double-nozzle electrospinning technique. It has been found that in such fibers, Si particles are encapsulated by the carbon shell of fibers, which can settle the shortcomings of pulverization and volume variation of Si. Furthermore, the highly conductive N–C shell derived from carbonized PAN can accelerate the diffusion of Li+ and charge transport. As a result, the as-prepared core–shell SC-NF-0.24 electrode exhibits an initial specific discharge capacity of 1441 mAh g–1 with a high capacity retention of 76.9% at 0.5 A g–1, and the capacity decay rate of per cycle is only 0.1% (starting on the third cycle), showing a good cycle property. Therefore, the as-prepared freestanding core–shell SC-NF material is a prospective anode material for high-performance lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
纳米科技
·
能源存储
·
功能材料
·
复合材料
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Fangkun Xiao,Haochen Ge,Yanyi Wang,Shengjun Bian,Yunbo Tong,Congjie Gao,Guiru Zhu
Polyethylene (PE) has recently gained attention as an advantageous support material in forward osmosis (FO) owing to its low structural parameters. A novel thin-film composite (TFC) membrane for FO was fabricated by introducing a tannic acid (TA)-Fe 3+ interlayer on a polydopamine (PDA)-modified PE support via interfacial polymerization. The TA-Fe 3+ interlayer influenced the diffusion of m -phenylenediamine, causing a unique worm-like morphology of the polyamide (PA) layer, distinct from the traditional “ridge and valley” morphology. Worm-like structures provided more permeation sites and improved the water flux (71.2 L⋅m −2 ⋅h −1 ). Furthermore, the TA-Fe 3+ interlayer prevented some salt molecules from passing through and resulted in a low specific salt flux (0.03 g⋅L −1 ). The TA-Fe 3+ interlayer was the key to overcoming the trade-off between permeability and selectivity. It functioned as a bridge connecting the PA layer and the PDA-modified PE support through chemical bonding, and the adhesion strength between PA layer and PDA-modified PE support was enhanced. This resulted in the excellent stability of the obtained TFC membrane. This study presents a new method for the design of a TFC membrane with excellent perm-selectivity and manipulatable morphologies of the PA layer for FO applications.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Niu Liu,Dongfang Guo,Shiwang Gao,Hanming Liu,Hongwei Niu,Lianbo Liu,Shiqing Wang,Qi Wang,Huanjun Wang,Wei Xu,Hongjun Zhang
To elucidate the direct air capture (DAC) performance and CO 2 selective sieving mechanisms of distinct porous materials under trace CO 2 conditions, three types of materials, anion-pillared materials, open site MOFs, and amine-modified materials, were synthesized, with their DAC performance systematically characterized. DFT-D3 calculations revealed that in NbOFFiVE-1-Ni, the C···F distances (3.04 Å) between CO 2 and the pillared NbOF₅ 2− anions, as well as the O···H distances (2.89 Å) between CO 2 and pyrazine linker hydrogens, are shorter than those in SIFSIX-3-Ni and GEFSIX-3-Ni. These synergistic C···F van der Waals (vdW) and O···H hydrogen-bonding interactions afford NbOFFiVE-1-Ni the highest CO 2 binding energy (62.74 kJ/mol), exceeding that of SIFSIX-3-Ni (57.79 kJ/mol), GEFSIX-3-Ni (60.47 kJ/mol), and MIL-101(Cr) (22.86 kJ/mol). Consistently, NbOFFiVE-1-Ni exhibits the highest atmospheric CO 2 uptake (1.15 mmol/g) among these materials. Given the low atmospheric CO 2 uptake of pristine MIL-101(Cr), two amines (PEI and TEPA) were used to modify it, leveraging its abundant unsaturated metal sites to enhance CO 2 adsorption capacity. DAC performance of amine-modified MIL-101(Cr) first increased then decreased with amine loading, with optimal values of 2.07 mmol/g (50 wt% TEPA) and 1.52 mmol/g (70 wt% PEI). DFT-D3 calculations demonstrated that TEPA molecules and PEI chains bind directly to the unsaturated metal sites of MIL-101(Cr), forming tadpole-like amine-modified MOF structures with binding energies of 210.01 kJ/mol and 178.30 kJ/mol, respectively. Positron annihilation lifetime spectroscopy (PALS) confirmed that TEPA incorporation generates new cavities, microporous structures, and abundant active amine sites in MIL-101(Cr) crystals, synergistically enhancing its DAC performance.
研究领域:
材料科学
·
环境化学
·
物理化学
·
多孔材料
·
碳捕集
✓ 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）