JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Zhihong Lin,Ziyi Yuan,Kaifang Wang,Xuezhong He
Novel mixed matrix membranes (MMMs) with superior CO 2 /N 2 separation properties are of great importance for post-combustion CO 2 capture from flue gas . Metal-organic frameworks (MOFs) as one of the most attractive porous fillers for MMMs fabrication, are considered to provide a solid molecular sieving mechanism for enhancing CO 2 /N 2 selectivity. However, it causes the reduction in gas permeability and limits its further industrialization. Herein, we proposed a new strategy for filler functionalization by doping silver ions (Ag + ) into UiO-66-NH 2 nanoparticles through the double-solvent method and used for the preparation of advanced MMMs. The double-solvent method is benefits for the enrichment of Ag + in the hydrophilic pores of UiO-66-NH 2 . As a result, the prepared novel MMMs called Ag + @UiO@PIM-1 with the polymers of intrinsic microporosity (PIMs) as polymer matrix , show outstanding CO 2 permeability. According to the mixed gases (CO 2 /N 2 = 10:90) permeation experiments under 25 °C and 2 bar, the membrane with 30%Ag + @10%UiO loading achieves more than 65% increase in CO 2 /N 2 selectivity (∼30) and 120% in CO 2 permeability (>15,000 Barrer) compared to the pristine PIM-1 membrane. By optimizing the Ag + doping amount and Ag + @UiO loading content, the separation performance exceeds the 2019 CO 2 /N 2 upper bound. To figure out the separation mechanism, the pore texture properties and CO 2 affinity of the functional filler (Ag + @UiO) together with the membrane structure were characterized by XPS , PXRD , SEM, gas sorption , etc. The synergistic mechanisms by combing CO 2 facilitated transport and molecular sieving from pore regulation were identified to enable advanced CO 2 /N 2 membrane separation .
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ACS Catalysis
·
2023
·
IF 12.9
Yanfei Liu,Zhang Liu,Chengxiong Wang,Jie Xu,Jianping Ai,Xiao Liu,Aimin Zhang,Yunkun Zhao,Chun Du,Bin Shan
Supported Pt catalysts suffer from low reaction selectivity (<65% at 100% conversion) in the selective catalytic oxidation of ammonia (NH3-SCO) because of their intrinsic over-oxidation tendencies. Herein, a strategy based on facilitating byproduct NOx reduction to N2 is demonstrated at CuOx/PtCu catalysts, aiming to tackle the low selectivity challenge. This PtCu alloy sample with a CuOx-rich surface displays an N2 selectivity of 95%, while its turnover frequencies are the highest among reported supported Pt-based catalysts. The enhanced reaction activities and N2 selectivities are primarily attributed to the Pt-Cuδ+ dual-site synergies at the CuOx/PtCu interface, in which dual sites exhibit distinct NH3 adsorption, activation, and dehydrogenation behaviors. The Olat assisted internal selective catalytic reduction mechanism at CuOx/PtCu with N2O22– as the central intermediates is proposed. Density functional theory calculation and temperature-programmed surface reaction measurements show that the N–O bond in N2O22– tends to break simultaneously with the assistance of Ov in CuOx followed by the easy transition from N2O22– to N2, which serve as the origin of the high selectivity.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Yuxiu Sun,Yunshuo Gao,Chenxu Geng,Zhengqing Zhang,Zhihua Qiao,Chongli Zhong
Metal-organic frameworks (MOFs), as a typical type of porous materials, are widely used as fillers in mixed matrix membranes (MMMs) to enhance the gas separation performance. However, non-selective interface defects are prone to appear in MMMs under high MOF loading conditions, meanwhile, the discontinuous dispersion of MOF particles in polymeric matrices makes the gas molecules diffuse along the MOF-polymer-MOF intersection path and difficult to achieve efficient molecular transfer. These factors greatly compromise the ability of MOF to enhance membrane separation performance. Herein, the [C 5 min][BF 4 ] encapsulated ZIF-67 (IL@ZIF) composites were embedded into the defect-free IL/Pebax ion gel matrix to form a mixed matrix ion gel membrane without interface defects. On the basis of good interfacial compatibility, the relatively continuous and highly selective CO 2 transmission channels were constructed via increasing the filler loading up to 80 wt%. In this context, the typical IL@ZIF/IL/Pebax membrane with 80 wt% IL content and 70 wt% IL@ZIF doping amount exhibits a CO 2 permeability of 408.2 Barrer and CO 2 /N 2 selectivity of 97.2, surpassing the latest upper line. This work may have high reference value in the construction and preparation of MOF-based MMMs with high performance in gas separation.
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RSC Advances
·
2016
·Vol. 6
·期 107
·105338-105346
·
IF 3.289
Deyuan Xie,Ye Sun,Tianle Zhu,Xing Fan,Xiaowei Hong,Wenhao Yang
NH3 synthesis from H2O + N2, H2 + N2 or H2O + H2 + N2 by dielectric barrier discharge combined with an Ru/Al2O3 catalyst is studied at atmospheric pressure and room temperature. Additionally, the effects of reaction gas composition, energy density, and discharge frequency on NH3 yield and by-product formation are investigated. The results show that NH3 can be formed from reaction gases consisting of H2O and N2. The NH3 yield of the reaction gas containing H2 is much higher than that of the reaction gas consisting of H2O and N2. The presence of H2O has a promotion effect on NH3 synthesis from H2 and N2, especially for reaction gases with an H2 content less than 10%. The NH3 yield first increases and then decreases with an increase in the energy density. The maximum yield of 680 mg kW−1 h−1 occurs at the energy density of 1400 J L−1 and in the reaction gas of 0.14% H2O, 40% H2 and N2. The discharge frequency has a great effect on the NH3 yield, and maximum NH3 yield is obtained at the frequency of 13 kHz. Besides NH3, some by-products, such as N2O and NO2, are also formed with reaction gases containing H2O. However, their formation can be suppressed in the presence of H2, which is attributed to the reduction effect of H2 on the by-products.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chunran Zhao,Chenrui Wang,Xujie Ren,Shude Yuan,Leihong Zhao,Lvchao Zhuang,Botao Teng,Ying Wu,Yiming He
Fabricating heterophase junctions proves to be an efficient strategy for achieving efficient charge separation and enhancing the catalytic activity of photocatalysts. Surprisingly, this approach is rarely utilized in the field of piezocatalysis. In this work, a novel ZnSnO 3 heterophase junction catalyst was fabricated by combining rhombohedral (R-ZnSnO 3 ) and orthorhombic (O-ZnSnO 3 ) phases for efficient piezo and piezo-photocatalytic RhB degradation and N 2 fixation. The piezocatalytic RhB degradation rates of ZnSnO 3 heterophase catalysts are 5.6 and 3.6 times higher than those of O-ZnSnO 3 and R-ZnSnO 3 , respectively, with similar enhancements observed in piezocatalytic N 2 fixation. The coupling of R-ZnSnO 3 and O-ZnSnO 3 does not increase the piezoelectric properties; however, an S-scheme structure formed at the interface. Under the combined effects of band bending, interface electric fields, and Coulomb attraction, electrons and holes migrate and achieve effective spatial separation. This result supports the energy band theory over the induction charge theory, contributing to the ongoing debate in piezocatalytic mechanisms. Electrochemical analyses and piezo-photocatalytic tests further indicate that ZnSnO 3 heterophase junctions exhibit a synergistic effect between piezocatalysis and photocatalysis. This synergy can be attributed to the complementary effects of photoinduced carrier generation and piezoelectric field-assisted carrier separation. Hydroxyl radicals, superoxide radicals, and holes serve as the primary active species responsible for piezocatalytic RhB degradation through a mechanism similar to photocatalysis. Theoretical calculations reveal that the Sn site on the surface of O-ZnSnO 3 acts as the active site within the ZnSnO 3 heterophase junction, providing valuable insights for future catalyst development. This work offers a deeper understanding of the synergistic mechanisms in piezo-photocatalysis, presenting a promising route for efficient environmental and energy applications.
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LANGMUIR
·
2025
·
IF 3.9
Xiao Zhang,Menglin Zhang,Zhiren Guo,Xiang Li,Ting Liu,Jinying Li,Dongxiang Zhang,Xiyan Xu
The persistent contamination of aquatic environments by tetracycline (TC) necessitates advanced remediation strategies. Herein, a ternary Fe–O–P-co-modified graphitic carbon nitride (FOPCNx) was synthesized via structural integration of Fe–N2 configurations with O/P dual doping for efficient TC degradation in a solar-driven photo-Fenton system. This study pioneers the synergistic coupling of Fe–N2 coordination and heteroatomic O/P substitution to optimize charge dynamics. Comprehensive characterization confirmed the formation of Fe–N2 active sites and aromatic structures incorporated with the aromatic group, which collectively enhanced visible-light absorption, suppressed electron–hole recombination, and facilitated charge carrier redistribution. The optimized FOPCN2 demonstrated exceptional photoelectric efficiency (3.7-fold higher photocurrent density than pristine g-C3N4) and achieved 98.9% TC removal within 40 min of irradiation with a kinetic constant of 0.113 min–1, outperforming conventional systems. Mechanistic studies revealed dual enhancement pathways: Fe–N2 sites promoted electron transfer and Fe(III)/Fe(II) cycling, while the O/P dual doping enabled electron delocalization for improved charge mobility. The system exhibited remarkable pH adaptability (3–7), robust resistance to inorganic anions, and universal degradation capability for mixed organic pollutants. Three TC degradation pathways were identified through intermediate analysis, with radical trapping and EPR verification confirming the dominant roles of •OH, e–, and O2•–. This work provides critical insights into structure–activity relationships for carbon nitride modification, establishing a paradigm for designing multifunctional photocatalysts for antibiotic-contaminated wastewater remediation.
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PubMed
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Advanced Sustainable Systems
·
2024
·
IF 6.5
Jiawei Zhou,Ming Liu,Shiyang Bai,Jihong Sun,Jia Wei,Ju Wang
The MOF-5@clinoptilolite (MOF@CP) composites are successfully synthesized using polyvinylpyrrolidone (PVP) for adsorption separation of CO 2 /CH 4 , CO 2 /N 2 , and CH 4 /N 2 . The effects of the PVP amounts on the dispersity of MOF-5 on CP random lamellas of the MOF@CPs are evaluated via various characterizations. Meanwhile, their single-component gas adsorption isotherms, breakthrough experiments, and cycling test are measured. The results elucidate that the used PVP amount has a significant influence on the particle size and the uniformity of MOF-5 dispersed on CP random lamellas. The MOF-5-loaded amount in MOF@CP is estimated to be up to 42.52 wt.%. Especially, the surface fractal evolutions indicated the surfaces of MOF@CP became from rough to smooth with the increase of PVP. The CO 2 /CH 4 , CO 2 /N 2 , and CH 4 /N 2 selectivity factors of MOF@CP are higher than that of CP, displaying a better separation performance. Their cycling test revealed that MOF@CPs could be used repetitively, highlighting efficiency for CO 2 and CH 4 separation. Meanwhile, the MOF-5@CP stability under moisture is preliminarily investigated, showing higher moisture resistance stability than MOF-5. Additionally, the grand canonical Monte Carlo simulations demonstrated the adsorption separation mechanism of the prepared MOF@CPs.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·
IF 3.8
Shuangjiang He,Junchang Wang,Chong Wang,Xiao Zhang,Sen Liang
The Mn-Fe-Co-Zn-O series is a widely used thermistor material, but its thermal stability is compromised by nitrogen glass encapsulation, limiting its application in electrical devices. To address this issue, La 2 O 3 and Y 2 O 3 were used as rare earth oxide dopants, and xR 2 O 3 -Mn 0.76 Fe 0.87 Co 1.07 Zn 0.3 O 4 (x = 0.0025, 0.005, 0.01, 0.02) negative temperature coefficient (NTC) materials were synthesized via solid-state sintering. The effect of rare earth doping on the electrical properties after high-temperature nitrogen annealing was investigated. After annealing at 750°C for 4 h, the variation in resistivity ( ρ 25 ) and material constant ( B 25/50 ) significantly decreases with increasing La doping. For the La-doped sample (x = 0.01), Δρ 25 decreased to 7.77% and ΔB 25/50 to 0.77% (for the Y-doped sample (x = 0.01), Δρ 25 decreased to 22.76% and ΔB 25/50 to 1.91%), compared to the undoped sample, where Δρ 25 reduced by 168.84% and ΔB 25/5 0 by 5.57%. This improvement was attributed to rare earth accumulation at grain boundaries, filling voids and forming R-O bonds, which inhibited oxygen vacancy migration and significantly reduced grain boundary resistance. Rare earth doping effectively improved the thermal stability and electrical consistency of NTC thermistor ceramics in high-temperature nitrogen atmospheres, offering a new strategy for high-temperature encapsulation applications. (Y-doped samples showed similar results, as detailed in the Supplementary Materials.)
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ENERGY & FUELS
·
2023
·
IF 5.3
Xiaojun Dai,Yan Cheng,Tingting Liu,Lingjuan Mao,Qiang Wei,Yasong Zhou
SAPO-11 molecular sieves with different crystal sizes and particle sizes, especially nanosized small-crystal SAPO-11 molecular sieves, were successfully synthesized, and the corresponding NiWS-supported catalysts were prepared for the hydroisomerization of n-hexadecane. XRD, SEM, N2 adsorption–desorption, Py-IR, and HRTEM were used to analyze the effects of crystal size and particle size of the supports on their physicochemical properties, active phase properties, and catalytic performance of the catalysts. Through reaction evaluation and analysis of isomeric products, the effects of the size change of the support on the hydroisomerization performance of the catalyst and the hydroisomerization depth of n-hexadecane were determined. Through comprehensive analysis of the cracking products, it was determined that secondary cracking occurred when the conversion of n-hexadecane on the NiW/SAPO-11-S catalyst reached about 42.7%, and the secondary isomerization occurred when the conversion of n-hexadecane reached about 80%. The hydroisomerization reaction network of n-hexadecane over the NiWS/SAPO-11 catalyst was studied emphatically, and it was found for the first time that the secondary cracking of n-hexadecane during hydroisomerization followed the C3-β-scission mechanism.
研究领域:
化学工程
·
催化
·
材料科学
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2013
·
IF 2.004
Chao Chen,Xiao-Sen Li,Zhao-Yang Chen,Zhi-Ming Xia,Ke-Feng Yan,Jing Cai
The equilibrium hydrate formation conditions for ternary simulated flue gas [CO2 (0.1368) + N2 (0.8547) + SO2 (0.0085)] with SO2 aqueous solutions, and SO2 + tetra-n-butyl ammonium bromide (TBAB) aqueous solutions were measured using the temperature search method, over the temperature and pressure range of (272.85 to 283.15) K and (1.20 to 5.09) MPa, respectively. The corresponding equilibrium gas compositions were analyzed. The effects of SO2 concentration and TBAB additive on the hydrate phase equilibrium were studied. For the flue gas and SO2 aqueous solution, the presence of SO2 reduces the hydrate formation pressure. The higher is the SO2 concentration in aqueous solution, the easier the hydrate forms, and the higher the SO2 concentration in equilibrium gas phase is. N2 mole fractions in equilibrium gas phase are higher than that in the feed flue gas, while CO2 is lower due to its relative high solubility. For a given system, the equilibrium hydrates formation pressure increases with the increase in temperature. Both SO2 and N2 mole fractions in equilibrium gas phase decrease with the increase in pressure, while the CO2 mole fraction increases. TBAB solution with w4 = 0.050 not only reduces the equilibrium hydrates formation pressure markedly, but also helps the dissolution of SO2 in aqueous solution. The SO2 concentrations in equilibrium gas phase for the TBAB addition system are much smaller than those without TBAB addition. The pressure reducing effect of the TBAB promoter for SO2 containing flue gas is dependent on the SO2 concentration and smaller than that for flue gas without SO2. A small amount of SO2 produces a synergy with TBAB to promote the hydrate formation, but the high SO2 concentration produces an inhibition on the hydrate formation, and causes the hydrate equilibrium pressure increase. The optimum SO2 mass fraction in solution is lower than 0.010.
研究领域:
化学工程
·
环境科学
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fanhui Meng,Lina Wang,Muhammad Asif Nawaz,Qian Wang,Zhiyuan Gong,Zhong Li
Direct conversion of syngas to light hydrocarbons has been intensively studied in recent years; however, the high selectivity of light hydrocarbons is still a challenging task to achieve a high CO conversion. Here, a bifunctional catalyst consisting of a methanol synthesis catalyst (CZA) and a methanol to dimethyl ether (DME) catalyst (Al 2 O 3 ) was employed with a hydrocarbon synthesis catalyst (SAPO-34), for syngas conversion to light hydrocarbons in a dual fixed-bed reactor. The conversion of simulated intermediates CO/CO 2 /DME/N 2 /H 2 with a molar ratio of 9/6/4/5/76, obtained from syngas conversion to DME over CZA and Al 2 O 3 , was studied over SAPO-34 zeolites. It was found that SP34-0.1 with Si/Al ratio of 0.1, exhibited low amount of strong acid (0.60 mmol/g) and high selectivity to light olefins (74.1%), while SP34-0.4 with Si/Al ratio of 0.4 exhibited high amount of strong acid (1.00 mmol/g) leading to high selectivity of light paraffins (88.4%). The in-situ DRIFTS analysis illustrated that DME can be rapidly adsorbed on the hydroxyl site of SAPO-34 and decomposed into the surface methyl species, where SP34-0.4 could produce more dimethylcyclopentenyl cationic species than SP34-0.1. It was suggested that the overall reaction route led to a high selectivity to light olefins (84.2%) with a CO conversion of 61.2% on (CZA + Al 2 O 3 ) catalyst combined with SP34-0.1, while a high selectivity to light paraffins (76.3%) could be achieved by combining with SP34-0.4 at 70.3% CO conversion. Since, the current study interprets that the selectivity of hydrocarbons can be adjusted by regulating the acidity of SAPO-34 to achieve a high CO conversion in the dual fixed-bed reactor scheme.
研究领域:
化学工程
·
催化科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xinyuan Wang,Zhuohang Wu,Taozhen Li,Xiaoning Wang,Pijun Duan,Jingwen Pan,Lei Wang
Sulfonamide antibiotics are highly toxic, persistent, and environmentally hazardous, necessitating effective remediation technologies for their removal from aquatic systems. Singlet oxygen ( 1 O 2 ), a selective and pH-tolerant reactive species, has emerged as a key oxidant in persulfate-based advanced oxidation processes (PS-AOPs). Herein, the systematic and novel pathway formation for the 1 O 2 on single Cu atom during PS-AOPs was elucidated. Nitrogen-doped biochar-supported single-atom Cu catalysts featuring low-coordination Cu-N 2 sites (SACu-N 2 @C) were synthesized via calcinating straw biomass, which showed remarkable catalytic efficiency towards sulfamethoxazole (SMX) oxidation even under high-salinity conditions. Results and further elucidated the 1 O 2 formation pathway, where the Cu-N 2 sites adsorbed and interacted the oxygen atom in S O group at the end of peroxymonosulfate (PMS) with lower adsorption energy. This process was accompanied by the generation of two SO 5 •− molecular intermediates, ultimately leading to the formation of 1 O 2 with the lowest energy barrier. Moreover, toxicity tests showed that the degraded SMX solution was ecologically safe with no significant toxic effects on zebrafish, rice and Escherichia coli ( E. coli ). This study provides atomic-level insights into 1 O 2 generation via Cu-N 2 coordination, advancing the design of efficient and environmentally benign Fenton-like systems for antibiotic wastewater treatment.
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