RSC Advances
·
2016
·Vol. 6
·期 55
·50138-50143
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IF 3.289
D. Li,W. B. Li,J. S. Shi,F. W. Xin
Hexagonally packed mesoporous silica (HMS) was used as a kind of template-like material to prepare heteroatom doped porous carbons from the polymerization reactions of resorcinol and formaldehyde in the HMS pore channels. Different acids (HNO3, H2SO4, H3PO4) were used to catalyze the polymerization reactions to obtain N-doped, S-doped, and P-doped porous carbons, respectively. The adsorption properties of H2, CH4, and CO2 were investigated on these doped carbon materials systematically. For the hydrogen adsorption, the adsorption amount was 11.8%, 21.1%, and 33.3% higher on N-doped, S-doped, and P-doped porous carbons, respectively, than the carbon sample without doping, and the highest hydrogen uptake reached 14.88 mmol g−1 on the P-doped sample; regarding the CO2 adsorption, the adsorption amount reached 3.60 mmol g−1 and 3.16 mmol g−1 on the S-doped sample and N-doped sample, respectively, which is 39.5% and 22.5% higher than the sample without doping; it also shows that methane uptake amount was significantly increased by 27.1% on the S-doped sample as compared to the sample without doping, i.e., 3.52 mmol g−1 of CH4. Therefore, it is predicted that these doped carbon materials with high specific surface area are of great potential for the gas adsorption of H2, CH4, and CO2.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2013
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IF 3.548
Zebao Rui,Danyan Feng,Huayao Chen,Hongbing Ji
Highly-ordered TiO 2 nanotube array (TiNT) was prepared by an electrochemical anodization method and used as the support for Ni and Ni–M (M = Ru, Pt and Rh) bimetallic catalysts . Ni/TiNT and Ni–M/TiNT were then applied to the combination reactions of the partial oxidation of methane reaction (POM) with the carbon dioxide reforming with methane reaction (CRM) for the syngas production . The results show that Ni/TiNT suffers from the formation of NiO and NiTiO 3 , and the coke deposition. The superior catalytic performance and the enhanced resistance ability against carbon formation are obtained over a small amount of noble metal modified Ni bimetallic catalysts, which are ranked as Ni/TiNT < Ni–Ru/TiNT < Ni–Pt/TiNT < Ni–Rh/TiNT. The interaction of Ni–M, i.e., enhanced reducibility of NiO and the maintenance of metallic Ni species even in the presence of oxygen, over Ni bimetallic catalysts is regarded as an important reason. Much short distance between the exothermic and the endothermic zones over Ni–M/TiNT catalysts bed can be realized, and a flat temperature profile in the catalyst bed is expected, which in turn can relieve the hot-spot and NiTiO 3 formation to some extent.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yating Xie,Nicui Yuan,Hongyang Liu,Lukai Luo,Jun Gong,Xiping Yin,Tengfei Li,Yonghua Zhou
Defect engineering by creating oxygen vacancies (OVs) and heterogeneous frustrated Lewis acid-base pairs (FLPs) emerged as an efficient strategy to enhance the selective conversion CO 2 to CH 4 . Considering the intrinsic FLPs contained in UiO-66-NH 2 (UNH for abbreviation), in this paper, the OVs was introduced therein by fabricating the Ce-doped UNH (denoted as UNH(Ce/Zr)) via one-step solvothermal route. The as-prepared UNH(Ce/Zr) catalyst exhibited the CH 4 yield of 31.02 μmol·g −1 ·h −1 accompanied with the CH 4 selectivity of 93 % and satisfying recycling stability. The XRD, SEM, FT-IR, XPS, TG, TPD and NH 3 in situ DRIFTS and in situ FT-IR characterization results justified that the UNH(Ce/Zr) possess the obviously increased OVs sites and enhanced Lewis acidic and basic properties. Additionally, the photoelectrochemical characterization results showed that UNH(Ce/Zr)−0.014 efficiently improved photogenerated electron-hole separation efficiency and charge transfer rate. It could be concluded that it was the cooperative action of OVs and FLPs that led to the high CH 4 selectivity and CH 4 yield.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhiwei Zhao,Yuan Li,Yanjie Wang,Yating Wang,Yuhao Tang,Mengyue Lu,Xu Yang,Xiaoqing Wang,Feifei Zhang,Jinping Li,Jiangfeng Yang
The enrichment of low-concentration coal-bed methane is beneficial to solving the world’s energy concerns. However, most adsorbents used for CH 4 /N 2 separation from coal-bed methane are hydrophilic and ineffective under humid conditions. In this study, a hydrophobic nickel-based metal–organic framework (TUTQ-1Ni) was developed for efficient CH 4 /N 2 separation under humid conditions. Adsorption results show that, at 298 K and 1 bar, TUTQ-1Ni exhibits the highest CH 4 /N 2 selectivity (11.0) among the reported hydrophobic CH 4 -selective metal–organic frameworks. The results of theoretical calculations reveal that multiple O/S sites provide strong adsorption affinity for CH 4 over N 2 . Further, breakthrough experiments confirm the suitability of the material for CH 4 /N 2 separation, with the separation performance being maintained at even a high relative humidity of 100 %. The pressure swing adsorption simulation results indicate that TUTQ-1Ni is a potential candidate material for the selective capture of methane from coal-bed methane.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Long Tian,Xinyou Han,Xiang Liu,Liangliang Zhang,Liping He,Xinyu Li,Zhuangzhuang Zhang,Dongyuan Yang,Binran Zhao,Chengyi Dai,Xiaoxun Ma
Nonthermal plasma (NTP) can convert CH4/H2O to high-value oxygen-containing chemicals (e.g., CH3OH) under mild conditions, but controlling product selectivity in this process remains a major challenge. Herein, a boron hydroxyl (B–OH)-rich catalyst (hereafter named BN/H2O2) was prepared via H2O2-assisted ball milling and found to regulate the yield and selectivity of the conversion of CH4/H2O to oxygen-containing compounds in an NTP reactor. A CH3OH yield of 1.04 mmol/h and a total carbon selectivity of 21.7% were achieved. BN/H2O2 showed approximately 2.6 and 1.5 times higher CH3OH yield and total carbon selectivity, respectively, than the hexagonal boron nitride catalyst. The results of sequential experiments and theoretical calculations indicated that the B–OH site at the nitrogen defect (VN) promoted the directed conversion of •CH3 to CH3OH via the Eley–Rideal mechanism, thereby enhancing the selectivity and yield of the conversion of CH4/H2O to CH3OH.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yanhu Han,Zhaowei Jia,Wenxue Gong,Xuechun Wei,Yu Zhang,Mengying Tao,Yaofei Ren,Zuyi Lu,Yutong Wu,Jianhua Chen,Zhongfeng Shi,Zhenxia Zhao,Zhongxing Zhao
Developing photocatalysts with high activity and selectivity remains a significant challenge in the field of CO 2 photoreduction for producing valuable chemical or fuel products under mild conditions. Herein, photonic crystal (PC) GDY-Cu/ZnO was constructed through the in-situ induced growth of graphdiyne (GDY) on PC Cu/ZnO surface via H 2 -reduction for efficient photoreduction of CO 2 to CH 4 . With the aid of photonic crystal structure, PC GDY-Cu/ZnO exhibits a distinctive red-edge slow light region which can significantly improve the utilization efficiency of visible light and intensify photo-catalysis. Additionally, the formed all-solid-state Z-scheme system efficiently accelerates photoelectron migration, facilitating e - /h + separation. Thirdly, the surface GDY, along with the enrich oxygen vacancies generated during H 2 reduction, enhances the adsorption and activation toward CO 2 and H 2 O on PC GDY-Cu/ZnO interface. In consequence, PC GDY-Cu/ZnO demonstrates highly photocatalytic conversion of CO 2 to CH 4 , achieving a CH 4 yield of 33.67 μmol·g −1 ·h −1 with 93.3 % selectivity via slow-light-driven photocatalysis CO 2 reduction. This work provides an efficient strategy to modify ZnO for the efficient photoreduction of CO 2 to CH 4 .
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zhihao Song,Xinrui Liu,De Ao,Zhihua Qiao,Zhi Wang,Song Zhao
Metal-organic framework glass shows great promise in gas separation applications, however, its inherent low porosity poses significant challenges to achieve the enhanced membrane permeability. In this work, we developed novel self-standing crystal-glass composite membrane via melt quenching process of porous organic cages and coordination polymer glasses. The resulting (CC3) n /( a g Zn-P-dmbIm) 1-n membranes effectively combines the high porosity of CC3 with the excellent film-forming property of Zn–P-dmbIm glass, enabling efficient CO 2 /CH 4 separation. Specifically, CO 2 molecules are preferentially adsorbed into the CC3 channels, followed by rapid permeation through the membrane, while the size exclusion restricts CH 4 molecules transport through the membranes. The obtained (CC3) 0.05 /( a g Zn-P-dmbIm) 0.95 membrane achieves a high CO 2 permeability of 9358 Barrer, a CO 2 /CH 4 selectivity of 24.2, and demonstrates 24-h operational stability. This study not only broadens the application scope of coordination polymer glasses in gas separation membranes but also provides novel insights for the design of high-performance crystal-glass composite membranes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yu Zhu,Liwei Lin,Man Zhou,Han Li,Yanan Wang,Song Xu,Zhongyu Li
The conversion of greenhouse gas CO 2 into usable high-value-added fuels through photocatalytic reactions is a promising green energy measure. However, the photocatalytic CO 2 reduction reaction faces challenges such as multi-electron transfer and slow mass transfer. Furthermore, most photocatalysts can only absorb ultraviolet light and have insufficient active sites, resulting in a low utilization rate of sunlight. Based on this, we designed a novel layered composite catalyst, where Ti 3 C 2 T x MXene serves as the supporting framework and BiOCl nanosheets are uniformly grown on its surface. Under simulated sunlight, the CH 4 yield is 30.07 μmol·g −1 ·h −1 , with a selectivity of 93.4 %, and it still maintains excellent stability after six photocatalytic cycle experiments. Research data indicates that with the intervention of reducing ethylene glycol, the oxygen vacancy content on Ti 3 C 2 T x /BiOCl is significantly increased. The formation of oxygen vacancies and Schottky heterojunctions not only enhances the charge separation efficiency at the interface but also selectively reduces CO 2 to CH 4 .
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SURFACE & COATINGS TECHNOLOGY
·
2024
·
IF 5.3
Tongguo Huo,Dan Zhu,Jianxin Zheng,Yuan Lin,Yu Dai,Jian Wu
This study systematically investigated for the first time the effects of varying the temperature, pressure, C/Si molar ratio, and H 2 /Si molar ratio on β-SiC coatings produced via chemical vapor deposition (CVD) using the SiCl 4 –CH 4 –H 2 –N 2 system. Thermodynamic theoretical calculations were performed using the HSC Chemistry software. The temperature and C/Si molar ratio considerably affected the morphology, phase, and composition of β-SiC coatings. High-quality β-SiC coatings along the (111) crystal plane exhibiting a uniform surface, high density, low roughness, and good crystallinity were successfully synthesized at 1523.15 K and 200 Pa with a C/Si molar ratio of 1.0 and H 2 /Si molar ratio of 6.5. Additionally, when N 2 was used as the dilution gas instead of Ar, the resulting β-SiC coatings demonstrated reduced roughness, fewer free carbon, increased hardness (37.05 GPa vs. 39.19 GPa), enhanced modulus of elasticity (237.26 GPa vs. 264.24 GPa), and superior coating adhesion (16.48 MPa vs. 18.29 MPa).
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Di Li,Qin Li,Yimeng Zhou,Qiong Zhang,Qianjin Ye,Ran Yang,Deli Jiang
Steering selectivity in photocatalytic conversion of CO2, especially toward deep reduction products, is vital to energy and environmental goals yet remains a great challenge. In this work, we demonstrate a facet-dependent photocatalytic selective reduction of CO2 to CH4 in Cu-doped TiO2 catalysts exposed with different facets synthesized by a topological transformation from MIL-125 (Ti) precursors. The optimized round cake-like Cu/TiO2 photocatalyst mainly exposed with the (001) facet exhibited a high photocatalytic CO2 reduction performance with a CH4 yield of 40.36 μmol g–1 h–1 with a selectivity of 94.1%, which are significantly higher than those of TiO2 (001) (4.70 μmol g–1 h–1 and 52.6%, respectively), Cu/TiO2 (001 + 101) (18.95 μmol g–1 h–1 and 69.6%, respectively), and Cu/TiO2 (101) (14.73 μmol g–1 h–1 and 78.9%, respectively). The results of experimental and theoretical calculations demonstrate that the Cu doping dominating the promoted separation and migration efficiencies of photogenerated charges and the preferential adsorption on (001) facets synergistically contribute to the selective reduction of CO2 to CH4. This work highlights the significance of synergy between facet engineering and ion doping in the design of high-performance photocatalysts with respect to selective reduction of CO2 to multielectron products.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Lili Gong,Ju Bai,Can Wang,Zhenyuan Li,Linglong Shan
Two-dimensional (2D) metal-organic framework (MOF) nanosheets are promising fillers for gas separation membranes, owing to their high aspect ratios and tunable pore architectures. Realizing their full application potential requires precise control over nanosheet morphology and sizes to optimize membrane performance. This work employs crystal growth kinetics modulation to tailor the morphology and size of ZIF-67-based nanosheets incorporated into mixed matrix membranes (MMMs) targeting superior CO 2 /CH 4 separation. Strategy (i): Adjusting early-stage nucleation kinetics yielded two distinct ZIF-L nanosheet types: disk-like (ZIF-L-I) and leaf-like (ZIF-L-II). ZIF-L-II, synthesized with higher ligand molar ratio, possessed larger lateral dimensions and more favorable pore characteristics, significantly enhancing gas separation. Strategy (ii): Amino-functionalized ionic liquid (IL) was introduced to further modulate the size of ZIF-L-II nanosheets. The IL's amino groups served as capping agents by coordinating preferentially with Co ions, restricting framework extension without altering crystallinity. The ILs loading amount dictated the final nanosheet size, but did not alter their crystalline phase. Critically, the IL also exhibits affinity for CO 2 , augmenting its transport. At 48 % IL addition, the CO 2 permeability of the 10 wt% IL-ZIF-L-II/PI membrane surged from 289 Barrer to 493 Barrer, without significant selectivity loss. The synergistic combination of kinetically-controlled synthesis (yielding larger and leaf-like nanosheets) and IL-mediated size regulation (providing both capping and CO 2 -philic functions) resulted in a 70 % enhancement in CO 2 permeability.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jiaqi Qiu,Mingnv Guo,Zhongqing Yang,Ziqi Wang,Ruiming Fang,Jiang He,Jingyu Ran
A series of novel iodine substitution and oxygen vacancy double defects Bi 2 MoO 6 nanosheets for enhanced photocatalytic reduction of CO 2 is reported, which exhibited superior CO 2 photocatalytic activity and CH 4 selectivity under full solar spectrum illumination. Bi 2 MoO 6 -I2 (the molar ratio of I to Mo is 0.13) has the highest photocatalytic activity, its CO yield is 2.0 times that of pure Bi 2 MoO 6 , the CH 4 yield is 12.2 times that of pure Bi 2 MoO 6 , and the CH 4 selectivity reaches 5.3 times that of pure Bi 2 MoO 6 . Its structure and physicochemical properties were investigated by material characterizations, photoelectrochemical tests and DFT calculations. The enhancement in CO 2 conversion and CH 4 selectivity benefit from: (1) Larger specific surface areas and smaller nanosheets thicknesses facilitate carrier migration; (2) More suitable band structure promotes the reduction of CO 2 ; (3) Insertion of impurity energy levels in the band gap enables efficient jumping of photogenerated electrons; (4) Double defects contribute to efficient CO 2 adsorption and activation; (5) Promoting highly selective conversion of CO 2 to CH 4 by optimising the formation energy of reaction intermediates.
研究领域:
材料科学
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环境科学
·
光催化
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