INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2013
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IF 2.206
Jiangfeng Yang,Junmin Li,Wei Wang,Libo Li,Jinping Li
Three hydrophobic microporous high-silica zeolites, DDR (with an 8-membered ring), silicalite-1 (a 10-membered ring), and beta (a 12-membered ring) were synthesized. The Si/Al ratios were 230, 1350, and 35, respectively. The samples were characterized by X-ray diffraction, scanning electron microscopy, thermal gravimetric analysis, water vapor adsorption, and volumetric nitrogen adsorption. They were tested for their CO2, CH4, and N2 adsorption properties at pressures of up to 10 bar at 288–313 K after activation, and the results were correlated with the Langmuir model. The heat of adsorption was calculated using the Clausius–Clapeyron equation based on the adsorption isotherms. These data were used to estimate the separation selectivities for CO2/CH4 and CH4/N2 binary mixtures at 298 K, using the ideal adsorbed solution theory (IAST) model. Experimental results showed that DDR and beta have good selectivities for CO2/CH4, because they have narrow pores (DDR) or more balance metal ions (relatively low Si/Al ratios beta) effect separately. The synthesized silicalite-1 has the lowest SCO2/CH4 but has the most suitable orifices for methane adsorption and the highest SCH4/N2. In addition, the breakthrough data for CH4/N2 mixtures further indicates that silicalite-1 is more suitable for the CH4 enrichment than the commercially used sorbents zeolite-5A and 13X. From the reproducibility of CH4 and N2 adsorption isotherms on silicalite-1, we can infer that which has the potential to be a commercial sorbent by the stable adsorption properties.
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高影响因子
Sustainable Materials and Technologies
·
2024
·
IF 8.6
Lei Guo,Yan-He Chen,Li-Mei Xu,Xiao-Lu Chen,Jin-Qiu Shen,Jian-Yong Zhang,Zhen-Jiang Liu
Herein, a fern-like p-n heterojunction by anchoring Ni 3 Fe-LDH nanoplates onto Co 3 O 4 nanoneedles have been optionally constructed. Essentially, p-n heterojunction ensured to induce strong built-in electric field, and inherit interfacial electron redistribution. Based on their compatible and well-matched electronic band structures, a staggered type-II photo-generated electron/holes transfer pathway have been elaborated by density functional theory calculation (DFT), in situ irradiation X-ray photoelectron spectroscopy (XPS), and fluorescent decay. This band bending and charge migrating module conferred the architecture with strong redox ability, sufficient exciton dissociation, and admirable optoelectronic characteristics. Moreover, the heterostructure acquired broad absorption spectrum to exhibit outperforming photocatalytic effect. Totally, this electron redistribution at the hierarchical interface, a type-II scheme charge-transfer pathway and the oxygen defects would lead to high efficiency in solar light assisted N 2 reduction. Typically, Co@Ni 3 Fe-2 catalyst exhibited the highest NH 3 production rate of 16.15 μg h −1 mg cat. −1 and Faraday efficiency (FE) of 31.57% at −0.6 V vs. RHE in 0.1 M Na 2 SO 4 solution. Fortunately, with light exposure, the NH 3 production rate and FE could increase by 27.9% and 18.1% than that under dark. This work would provide a plausible attitude towards the design of high efficient photocatalyst for artificial photosynthesis with multi-functionalized coupling effect.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Caifeng Xia,Qikang Yin,Xinle Sun,Qinglong Liu,Sen Liu,Shuxian Wei,Siyuan Liu,Weifeng Lv,Zhaojie Wang,Xiaoqing Lu
As a unique polymer of intrinsic microporosity, PIM-1 has great potential in mixed matrix membranes (MMMs) for gas separation with ultra-high permeability. However, the separation performance, e.g. CO 2 /N 2 separation, is still limited by its poor selectivity. In this work, PIM-1-based MMMs containing tartaric acid anion intercalated layered double hydroxides (TA-LDH) nanofillers are successfully prepared. The uniformly dispersed TA-LDH in the PIM-1 matrix contributes to optimizing the stacking of polymer chains for accessible pores, which is conducive to CO 2 diffusion. In addition, the assistant experiment and theoretical calculation point out that the -COO - , –OH between the TA-LDH layers had an affinity for CO 2 , creating a two-dimensional fast transport channel between the enlarged interlayer space. Compared with the pristine PIM-1 membrane, the CO 2 permeability and CO 2 /N 2 selectivity of 0.7 % TA-LDH/PIM-1 membrane is increased by 43.19 % and 105.48 %. The excellent gas separation performance with CO 2 permeability of 8343.18 Barrer and CO 2 /N 2 selectivity of 39.02 exceeds the 2019 Robson upper limit. This paves a new way to improve the gas separation performance of PIM-1-based MMMs and suggests high perspectives for real applications.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiaofeng Wang,Zhe Zhao,Yang Xu,Qingbo Li
A series of 3DOM-Mn x Ce y Ti z catalysts with three-dimensionally ordered macroporous (3DOM) structure were synthesized by a soft template method. The high SCR activity of the 3DOM-Mn 3 Ce 1 catalyst at low temperature was owing to the excellent redox ability and rich Lewis and Brønsted acid sites of the catalysts, which were beneficial to improve the catalytic activity. However, the strong oxidizability of MnO x resulted in the nonselective oxidation of NH 3 and generation of N 2 O, decreasing the N 2 selectivity. After addition of Ti, the redox capacity of the 3DOM-Mn 3 Ce 1 Ti 1 catalyst decreased, and the NH 3 were strongly adsorbed on the acid sites, which enhanced the N 2 selectivity with a broadened temperature window of 240–440 °C and a high GHSV of 120000 h −1 . Furthermore, both the 3DOM-Mn 3 Ce 1 and 3DOM-Mn 3 Ce 1 Ti 1 catalysts showed remarkable tolerance of H 2 O. Finally, through in situ DRIFT analysis, the Langmuir-Hinshelwood (L-H) mechanism was confirmed as the dominant reaction pathway over the 3DOM-Mn 3 Ce 1 Ti 1 catalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhiang Hou,Jiangfeng Chu,Cong Liu,Jinnan Wang,Aimin Li,Tong Lin,Corvini Philippe François-Xavier
Photocatalytic denitrification has attracted great attention owing to its high efficiency and environmentally friendly features. However, selectively photocatalytic reduction of high concentration nitrate to N 2 is still a challenging problem due to the competition of photons between nitrate and photocatalysts. Herein, the Ag/SiO 2 core encapsulated in the crystalline TiO 2 shell (Ag/SiO 2 @ c TiO 2 ) was constructed for improvement of photocatalytic denitrification. Finite difference time domain (FDTD) simulation demonstrated that strong light scattering improved light harvesting via optical confinement. Meanwhile, surface plasmon resonance and electron sink effect of Ag not only enhanced the photogenerated electrons density but also promoted charge carriers separation of Ag/SiO 2 @ c TiO 2 . More importantly, e cb − of TiO 2 -shell could be immediately transferred to Ag to keep the balance between Ag 0 and Ag + , which contributed to the good stability of Ag/SiO 2 @ c TiO 2 . 95.8% nitrate ( C 0 = 2000 mg/L) was removed by 5 wt%Ag/SiO 2 @ c TiO 2 with N 2 selectivity of 93.6% within 4 h. Even after five cycles, 5 wt%Ag/SiO 2 @ c TiO 2 still remained high photocatalytic denitrification efficiency (92.2%). Notably, since TiO 2 -shell prevented the reaction between Ag and Cl − , more than 92% nitrate could be removed within 5.3 h in the presence of high concentration Cl − .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Yang Li,Mingyuan Li,Zhihong Lin,Moris S. Eisen,Dario R. Dekel,Xuezhong He
An ultrathin amine-rich selective layer comprising the fixed-site carrier from polyvinylamine (PVAm) and the mobile carrier with an amino acid salt was successfully coated on top of the polysulfone (PSf) substrate for enhanced CO2-facilitated transport. PVAm with an ultrahigh molecular weight was synthesized via the inverse emulsion polymerization method, which allows the excellent dissipation of the reaction heat and reduces gel formation drastically. Several batches of PVAm with different hydrolysis degrees and molecular weights were successfully synthesized. The mobile carriers of 2-(1-piperazinyl)ethylamine salts of sarcosine (PZEA-Sar) were synthesized and introduced to strengthen the facilitated transport contribution, while cellulose nanocrystals (CNCs) were incorporated into the polymer matrix to enhance the mechanical strength and also increase the free volume of the polymer matrix. The amine-rich composite membranes made from 0.5 wt % PVAm/PZEA-Sar-0.5 wt % CNC with a high-molecular-weight PVAm of 4.4 MDa at a degree of hydrolysis (DOH) of 78% demonstrate a significantly enhanced CO2 permeance of 160 GPU with a good CO2/N2 selectivity of 48 at 35 °C and a feed pressure of 2 bar. The developed amine-rich facilitated transport membrane shows excellent potential for industrial carbon capture.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Chuanzhi Sun,Hao Liu,Wei Chen,Dezhan Chen,Shuohan Yu,Annai Liu,Lin Dong,Shuai Feng
A series of Sm- and/or Zr-doped MnO x -TiO 2 catalysts were prepared, and the catalysts exhibited better N 2 selectivity and SO 2 resistance than the undoped MnO x -TiO 2 catalyst for the selective catalytic reduction of NO by NH 3 (NH 3 -SCR). The reasons for the good N 2 selectivity and SO 2 resistance of the catalysts were proposed. X-ray photoelectron spectroscopy (XPS) combined with density functional theory (DFT) calculations suggested that electron transfer between the manganese and samarium species by Mn 4+ + Sm 2+ ↔ Mn 3+ + Sm 3+ redox cycles occurred in the Sm-containing catalysts. Furthermore, electron transfer from Sm 2+ to Mn 4+ suppressed electron transfer from NH 3 to Mn 4+ , inhibiting the formation of NH 2 or NH. Thus, the pathway for NH generation was removed, and the reaction of 2NH + 4NO → 3N 2 O + H 2 O was prevented. Consequently, the N 2 selectivity of the NH 3 -SCR reaction was enhanced. In situ diffused reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) combined with thermogravimetry, differential scanning calorimetry and mass spectrometry (TG-DSC-MS) results revealed that the deposition rate of sulfate species decreases after Sm doping, which was also attributed to the suppressed electron transfer from SO 2 to Mn 4+ , i.e., the oxidation of SO 2 to SO 3 . Thus, the catalysts exhibited better SO 2 resistance.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
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IF 7.149
Yan Zhang,Jinhua Li,Jing Bai,Linsen Li,Shuai Chen,Tingsheng Zhou,Jiachen Wang,Ligang Xia,Qunjie Xu,Baoxue Zhou
The conversion of excess ammonia N into harmless N2 is a primary challenge for wastewater treatment. We present here a method to generate ClO• directionally for quick and efficient decomposition of NH4+ N to N2. ClO• was produced and enhanced by a bifacial anode, a front WO3 photoanode and a rear Sb–SnO2 anode, in which HO• generated on WO3 reacts with HClO generated on Sb–SnO2 to form ClO•. Results show that the ammonia decomposition rate of Sb–SnO2/WO3 is 4.4 times than that of WO3 and 3.3 times than that of Sb–SnO2, with achievement of the removal of NH4+ N on Sb–SnO2/WO3 and WO3 being 99.2 and 58.3% in 90 min, respectively. This enhancement is attributed to the high rate constant of ClO• with NH4+ N, which is 2.8 and 34.8 times than those of Cl• and HO•, respectively. The steady-state concentration of ClO• (2.5 × 10–13 M) is 102 times those of HO• and Cl•, and this is further confirmed by kinetic simulations. In combination with the Pd–Cu/NF cathode to form a denitrification exhaustion system, Sb–SnO2/WO3 shows excellent total nitrogen removal (98.4%), which is more effective than WO3 (47.1%) in 90 min. This study provides new insight on the directed ClO• generation and its application on ammonia wastewater treatment.
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PubMed
高影响因子
Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 12
·2050-2060
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IF 4.5
Ren Jiahui,He Yongping,Sun Haidong,Zhang Rongzi,Li Juan,Ma Wenbiao,Liu Zhong,Li Jun,Du Xiao,Hao Xiaogang
Reducing the dissolution of Mn from LiMn 2 O 4 (LMO) and enhancing the stability of film electrodes are critical and challenging for Li + ions selective extraction via electrochemically switched ion exchange technology. In this work, we prepared a nitrogen-doped carbon cladding LMO (C-N@LMO) by polymerization of polypyrrole and high-temperature annealing in the N 2 gas to achieve the above purpose. The modified C-N@LMO film electrode exhibited lower Mn dissolution and better cyclic stability than the LMO film electrode. The dissolution ratio of Mn from the C-N@LMO film electrode decreased by 42% compared to the LMO film electrode after 10 cycles. The cladding layer not only acted as a protective layer but also functioned as a conductive shell, accelerating the migration rate of Li + ions. The intercalation equilibrium time of the C-N@LMO film electrode reached within an hour during the extraction of Li + ions, which was 33% less compared to the pure LMO film electrode. Meanwhile, the C-N@LMO film electrode retained evident selectivity toward Li + ions, and the separation factor was 118.38 for Li + toward Mg 2+ in simulated brine. Therefore, the C-N@LMO film electrode would be a promising candidate for the recovery of Li + ions from salt lakes.
研究领域:
材料科学
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电化学
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能源存储
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2022
·Vol. 39
·期 1
·315-324
·
IF 6.535
Qianjin Lin,Wanxiong Liao,Jia Cheng,Chun Zou,Bin Yang,Wenxiang Xia
Few studies on the low-temperature combustion behavior of MIPK, being a promising fuel additive , have been conducted. In this work, ignition delay times (IDTs) of MIPK were measured in the temperatures ranging between 780–910 K and pressures of 20 and 25 bar using a rapid compression machine (RCM). Oxy-fuel combustion combined with biofuel could remove CO 2 from the atmosphere. The IDTs of MIPK were measured in the temperatures ranging between 1125–1600 K under the O 2 /CO 2 atmosphere at the pressures of 1 and 10 bar using a shock tube . A low to high-temperature MIPK kinetic model (HUST-MIPK model) was proposed, in which the low-temperature sub-model consists of 19 low-temperature reaction classes and was constructed by analogy-based method, the high-temperature sub-model was adapted from the works of Cheng et al.. The predictions of HUST-MIPK model are in good agreement with the present low-temperature IDTs, high-temperature O 2 /CO 2 atmosphere IDTs, and the literature experimental data. The negative temperature coefficient (NTC) behavior was not observed in the temperature range from 790 to 910 K in the present RCM experiments, but was observed for methyl propyl ketone (MPK) and diethyl ketone (DEK) under similar conditions. The low-temperature chemistry of three pentanone isomers (MIPK, MPK, and DEK) was compared using the flux and sensitivity analysis. The comparison of the experimental high-temperature IDTs between O 2 /CO 2 and O 2 /Ar atmospheres indicates the IDTs of MIPK under O 2 /CO 2 atmosphere are longer than those under O 2 /Ar atmosphere at 1 bar, and the effects of CO 2 are almost independent of the pressure. The physical and chemical effects of CO 2 on the ignition were studied in detail.
研究领域:
燃烧化学
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燃料化学
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反应动力学
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能源工程
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大气环境影响
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Guangping Lei,Yang Lu,Zihan Liu,Yayun Zhang,Guojun Xi,Huiyuan Cheng,Wenji Rao,Xuhuan Guo
The greenhouse effect associated with excessive CO 2 emission has led to a series of environmental issues, thus developing excellent adsorbents for CO 2 capture from flue gas offers a sustainable approach. To combine the merit of multiple functional components, novel FeTPP@MIL-101(Cr) was prepared by incorporation of 5,10,15,20-tetrakis(4-methylphenyl)porphyrinato iron (III) chloride (FeTPP) into MIL-101(Cr) cages via in-situ packaging strategy. The cage-confined FeTPP can both regulate the pore structures of MIL-101(Cr) and provide additional binding sites for CO 2 adsorption. Profiting from extra interactions for CO 2 component and the “sieving effect” for N 2 component induced by incorporation of FeTPP, the discrepancy of isosteric heat for CO 2 and N 2 was largely amplified. Notably, the CO 2 /N 2 selectivity (15/85, v / v ) calculated by ideal adsorbed solution theory (IAST) increased from 17.1 (MIL-101 (Cr)) to 41.8 (FeTPP@MIL-101 (Cr) with FeTPP loading of 4.98 wt%) at 273 K, 100 kPa, which is 2.44 times larger than that of pristine MIL-101 (Cr) and also exceeds most reported adsorbents.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yixuan Zhang,Cong Liu,Ye Zhou,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Hollow double-shelled Ag@SrTiO 3 -TiO 2 with Z-scheme heterostructure was constructed for highly efficient photocatalytic reduction of nitrate to N 2 . The 3D finite-difference-time-domain analysis indicated that hollow double-shelled structure improved light harvesting due to multiple reflections. Photo-generated electrons transfer from SrTiO 3 to Ag 0 caused by electron sink effect were utilized to reduce nitrate, while photo-generated electrons of TiO 2 migrated to SrTiO 3 via transport bridge of Ti 3+ defects for electron–hole recombination. Such charge carriers migration pathway facilitated the construction of Z-scheme heterostructure, which enhanced charge separation yet still retained high redox powers. Both photogenerated electrons and CO 2 − played important role in photocatalytic denitrification. Furthermore, Ag 0 acted as co-catalyst which not only promoted photogenerated electrons transfer to nitrate but also enhanced nitrate conversion selectivity to N 2 . Combining the above advantages, nitrate removal rate and the nitrogen selectivity reached 97.2 % and 98.8 % within 60 min, respectively. Even after five cycles, it still remained satisfied photocatalytic activity and stability. In summary, this work proposed a feasible strategy to construct Z-scheme hollow double-shelled photocatalyst for efficient photocatalytic denitrification.
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