CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Minzhi Ma,Jiahao Chen,Zeai Huang,Wenjun Fa,Fang Wang,Yuehan Cao,Yuantao Yang,Zhiqiang Rao,Rui Wang,Ruiyang Zhang,Yanzhao Zou,Ying Zhou
Photocatalytic reduction of CO 2 with H 2 O to CH 4 is a promising route to migrate CO 2 emission and complete the carbon neutrality goal. Nevertheless, one of the biggest challenges for this elegant strategy is that the coupling of the protons and CO 2 to form CH 4 is fiercely competed with proton-proton coupling to form H 2 , leading to extremely low CH 4 selectivity. Herein, we designed and fabricated the nitrogen-doped carbon layers modified cobalt (N-C@Co) photocatalyst achieving the selective coupling of protons and CO 2 to CH 4 during photocatalytic reduction of CO 2 . The successful formation of intermolecular hydrogen bonds between the as-prepared N-C@Co and H 2 O molecule was found to suppress the mass transfer of the generated protons and promote the adsorption and activation of the CO 2 molecule. More crucially, it was conducive to suppressing the desorption of the CO intermediate, which was typically deemed as the decisive species for CH 4 generation. As a result, the H 2 selectivity (9.0 %) and activity (17.3 µmol g −1 ) of the as-prepared N-C@Co were reduced by a factor of 9.3 and 17.6, respectively, as compared to that of bulk Co. The CH 4 selectivity of N-C@Co was boosted 6.1 times from 13.3% of bulk Co to 81.3 % of N-C@Co with the generation rate of 155.7 μmol g −1 in 23 h. This work provides a new insight into the photocatalyst design for improving CH 4 selectivity and suppressing the competing H 2 and CO generation.
研究领域:
材料科学
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环境科学
·
催化化学
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2019
·
IF 2.298
Shuanshi Fan,Shali You,Yanhong Wang,Xuemei Lang,Chi Yu,Shenglong Wang,Zunzhao Li,Wentao Li,Yuanzhi Liu,Zheng Zhou
In this work, binary gas mixtures of 92 mol % CH4/CO2 and ternary gas mixtures of 87 mol % CH4/5 mol % C2H6/CO2 were studied as simulate associated petroleum gas. It mainly consists of two parts: one is the hydrate phase equilibrium of the binary and ternary gas mixtures both in water and 0.293 mol % tetra-n-butyl ammonium bromide (TBAB) solution by isochoric pressure-search method, and the other is the enthalpy of hydrate dissociation calculated by the Clausius–Clapeyron equation. The hydrate phase equilibrium measured temperature ranged from 278.61 to 289.46 K and pressure from 2.12 to 10.06 MPa with 24 points in total. The results show that the hydrate phase equilibrium line of 87 mol % CH4/5 mol % C2H6/CO2 + water was shifted about 2.4 K toward the higher temperature compared to that of 92 mol % CH4/CO2 + water. After adding 0.293 mol % TBAB, it could be found that the hydrate phase equilibrium line of binary gas mixtures and ternary gas mixtures in 0.293 mol % TBAB(aq) were shifted about 5.3 and 2.7 K toward the higher temperature compared to that of water. Besides, the enthalpy of the hydrate dissociation in 0.293 mol % TBAB(aq) is much higher than that in water. Average enthalpy of the hydrate dissociation of binary gas mixture hydrate increased from 62.46 kJ/mol in water to 160.21 kJ/mol in 0.0293 mol % TBAB(aq). Meanwhile the average enthalpy of hydrate dissociation of ternary gas mixture hydrate increased from 72.89 kJ/mol in water to 181.61 kJ/mol in 0.0293 mol % TBAB(aq).
研究领域:
化学工程
·
能源科学
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2026
·Vol. 37
·期 16
·1272
·
IF 3.2
D Subash T,Sukanya M.,Haripriya D.,Saranya K.,R Balaji S,Pandi V. Samuthira
Perovskite bilayer composites offer an effective approach for enhancing photocatalytic CO 2 reduction performance and operational stability under visible light irradiation. However, their practical implementation is limited by complex material design processes and difficulty in optimizing catalytic parameters for high selectivity. To address these issues, this paper gives an intelligent technique for photocatalytic CO 2 reduction to CH 4 with enhanced selectivity using 3D/2D perovskite bilayer composites. The proposed method integrates the Wasserstein Deep Convolutional Generative Adversarial Network (WDCGAN) with a Starfish Optimization Algorithm (SFOA). The main objective is to maximize CH 4 yield and selectivity while minimizing charge recombination losses in the photocatalytic process. The WDCGAN model is employed to predict photocatalytic activity based on material and structural features, while SFOA optimizes key catalyst parameters to achieve improved reaction performance. The proposed method demonstrates better performance than existing techniques, including the Genetic Algorithm (GA), Deep Neural Network (DNN) and Artificial Neural Network (ANN), as evaluated and compared using the MATLAB platform. The proposed SFOA-WDCGAN method demonstrates the highest R 2 of 0.99, accuracy of 99.5%, and efficiency of 98.5%, indicating improved performance compared to existing methods. The proposed strategy enables the design of stable and high-performance 3D/2D perovskite bilayer catalysts, significantly enhancing photocatalytic CO 2 reduction efficiency, CH 4 yield, and selectivity, making it promising for sustainable fuel generation applications.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2026
·Vol. 71
·期 8
·3669-3680
·
IF 2.4
Wu Shasha,Li Wenyu,Yang Li,Chen Zhen,Qin Yuanhang,Yuan Lunyong,Sun Wei
This study systematically investigates the influence
of lithium
nitrate (LiNO 3 ) modification on the gas adsorption characteristics
of UiO-66. The adsorption isotherms for carbon dioxide (CO 2 ), methane (CH 4 ), and nitrogen (N 2 ) were acquired
within a pressure range of 0 to 20 bar. The results from the cyclic
testing indicate that the UiO-66–0.05LiNO 3 variant
exhibits commendable stability. Notably, the incorporation of LiNO 3 enhances the CO 2 adsorption capacity by 29.48%,
reaching 2.24 mmol·g –1 at a pressure of 1 bar.
This is attributed to the introduction of lithium ions, which enhance
the electrostatic interaction between CO 2 and the MOF.
Analysis of the high-pressure data reveals that the Langmuir–Freundlich
model provides the most robust fit, whereas the Langmuir and Dual-site
Langmuir models demonstrate increased discrepancies as pressure escalates.
According to calculations based on the Ideal Adsorption Solution Theory
(IAST), the maximum selectivity of the material for the CO 2 /CH 4 and CO 2 /N 2 mixtures is 11.5
and 56.0, respectively. These results suggest that LiNO 3 modification significantly enhances both the adsorption capacity
and the selectivity for CO 2 separation.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Ruohan Xu,Ming Liu,Tallat Munir,Shiyang Bai,Jihong Sun,Haoqian Guo,Zhongchao Sun,Xiaoyan Bai
This study explores the preparation of the Ni-based catalysts supported on clinoptilolite (CP) for dry reforming of methane (DRM) using three methods: impregnation, complex route, and one-pot synthesis. The impact of these strategies on Ni dispersion and catalytic performance was investigated. Triethylamine was utilized as a complexing agent to improve Ni dispersion, prevent catalyst sintering, and reduce carbon deposition. The physicochemical properties were characterized using X-ray diffraction patterns, Fourier transform infrared spectroscopy, Raman spectra, and X-ray photoelectron spectroscopy spectra, N 2 adsorption–desorption isotherms, scanning electron microscopy and transmission electron microscopy images, hydrogen temperature-programmed reduction and thermogravimetric analysis. The results indicate that the CP-TEA/4Ni catalyst prepared via the complex route exhibited a higher Ni content (2.84 wt%) and demonstrated the highest initial activity at 600 °C (44.5% CH 4 conversion, 43.4% CO 2 conversion). Conversely, the (3NiTEA)CP catalyst synthesized via the one-pot method confined Ni particles within the microporous structures of CP, significantly suppressing carbon deposition and Ni particle growth, and thereby ensuring exceptional stability (105 h at 600 °C). The amorphous and graphitic carbon deposition coexisted in the deactivated catalysts, whereas the I D /I G value of the deactivated CP/TEA-3Ni was higher. Furthermore, Grand Canonical Monte Carlo-Molecular Dynamics coupled simulations revealed that surface Ni clusters were conducive to enhancing CH 4 adsorption heat and facilitating CO 2 diffusion, which effectively inhibited carbon deposition. These findings underscore the role of synthetic strategies in designing high-performance Ni-based catalysts for DRM reaction, offering pathways to more cost-effective, stable, and efficient catalysts for industrial methane reforming and carbon emission reduction.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
IF 3.5
Mi Yan,Cao Miao,Teng Cang,Xiangzhi Kong,Yan Zhang,Shuai Liu,Dan Wang,Ekkachai Kanchanatip
UiO-66 MOF was functionalized with dual ligands namely BDC-NH 2 and BDC-(OH) 2 . • Selective CO 2 /CH 4 adsorption were investigated at atmospheric and high pressures. • The highest CO 2 /CH 4 selectivity of 35.60 was achieved with 10%H-ZrMOF-A adsorbent. • CO 2 adsorption capacity of the adsorbent remained over 91.5% after five reuses. Selective CO 2 /CH 4 separation is essential for biogas valorization, yet conventional adsorbents typically face a trade-off between adsorption capacity and selectivity. In this work, a dual-ligand engineering strategy is implemented on UiO-66-NH 2 (ZrMOF-A) by co-incorporating 2,5-dihydroxyterephthalate (BDC-(OH) 2 ) to create a series of mixed-ligand MOFs denoted X %H-ZrMOF-A ( X = 5%–50% (mass)). The materials were synthesized via a solvothermal route and systematically characterized by N 2 physisorption, powder X-ray diffraction, FTIR spectroscopy, and SEM to elucidate structure-property relationships. Increasing hydroxyl content progressively modified surface area, pore volume, and morphology, with excessive BDC-(OH) 2 loading (>30% (mass)) inducing pronounced structural degradation. Among the series, 10%H-ZrMOF-A exhibited the most favorable balance between textural properties and functional site density, achieving a CO 2 uptake of 1.352 mmol·g –1 and a CO 2 /CH 4 selectivity of 35.60 at 100 kPa and 25 °C for a 40:60 CO 2 :CH 4 mixture predicted by IAST. Multi-model isotherm analysis identified the Freundlich and Elovich models as the most suitable descriptions of CO 2 adsorption, confirming a heterogeneous adsorption landscape arising from the coexistence of amine and hydroxyl sites. Complementary DFT calculations showed that dual functionalization strengthens CO 2 binding while weakening CH 4 interactions, consistent with the experimentally observed enhancement in selectivity. Pressure-dependent measurements revealed that high CO 2 /CH 4 selectivity at low pressures (≤100 kPa) diminishes at elevated pressures as non-selective pore filling becomes dominant, indicating that 10%H-ZrMOF-A is particularly suited for low-pressure biogas upgrading and post-combustion CO 2 capture. Five consecutive adsorption-desorption cycles demonstrated 91.5% capacity retention, confirming moderate short-term recyclability under mild thermal regeneration conditions. Download: Download high-res image (204KB) Download: Download full-size image
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Zecheng Lv,Enjun Zhu,Lanyun Wang,Yongliang Xu,Yuanwei Huang,Kun Zhang,Xiaodong Feng
H 2 + CH 4 hydrate is a promising solid state gas-storage medium, but its slow formation and limited stability under heating conditions restrict its practical application. In this study, 1,3-dioxolane (1,3-DIOX) and perfluorooctane (C 8 F 18 ) were used as single and combined additives for H 2 + CH 4 hydrate formation with a 25 mol% H 2 + 75 mol% CH 4 gas mixture. Their effects on phase equilibrium, nucleation, gas uptake, and heating-induced dissociation behavior were investigated. 1,3-DIOX acted as the dominant thermodynamic and kinetic promoter, yielding equilibrium temperatures of 291.05–293.75 K at pressures of 4.90–7.02 MPa and producing the highest gas uptake of 0.09781 mol/mol. In contrast, C 8 F 18 had limited influence on phase equilibrium and formation kinetics but delayed gas release during heating-induced dissociation. The combined system showed functional complementarity between formation promotion and dissociation-response regulation for H 2 + CH 4 hydrate storage.
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高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Qiangqiang Xue,Kang Hui Lim,Zhehao Sun,Binhang Yan,Zongyou Yin,Ange Nzihou,Yujun Wang,Guangsheng Luo,Feng-Shou Xiao,Sibudjing Kawi
Dry reforming of methane (DRM) over Ni-based catalysts is an economically reasonable technology for large-scale CO 2 utilization. However, prolonged Ni sintering and carbon deposition reduce the durability and efficiency of DRM, hindering its engineering application. Herein, we propose a facile approach by combining continuous microscale coprecipitation with solid-state reactions to construct a BaAl 2 O 4 -overlayer-confined Ni catalyst. The 5-wt.%-Ni@BaAl 2 O 4 catalyst exhibited advanced CO 2 and CH 4 conversions of 96% and 86% at 800 °C and a GHSV of 144 L∙g cat. −1 ∙h −1 . Moreover, the k d -CO 2 and k d -CH 4 of Ni@BaAl 2 O 4 were 0.0063 and 0.0029 h −1 ; which are approximately half and one-thirds of those of Ni/BaAl 2 O 4 and slightly better than those of Ni@MgAl 2 O 4 , underscoring the versatility of the proposed synthesis protocol for constructing core–shell structures. XAS, HAADF–STEM–EDS, and CO transmission-IR characterizations confirmed the SMSI of ∼2-nm amorphous BaAl 2 O 4 -overlaid ∼10 nm Ni with an overall mesoporous structure. After a long-term test, the sintering and coking inhibition effects of Ni@BaAl 2 O 4 (10 → 11 nm, 0.55 mg C ∙g cat. −1 ∙h −1 ) outperformed Ni/BaAl 2 O 4 (13 → 22 nm, 1.90 mg C ∙g cat. −1 ∙h −1 ) and Ni@MgAl 2 O 4 . In situ time-resolved CH 4 → CO 2 transient response, DRIFTS experiments, and DFT calculations suggested that Ni@BaAl 2 O 4 and Ni/BaAl 2 O 4 followed the Mars–van Krevelen and Langmuir–Hinshelwood redox mechanisms, respectively. The functional interfacial lattice oxygen promoted the removal of C ads * on Ni and core–shell structure induced fast CO 2 adsorption and CO desorption. The present study provides a facile approach for constructing a stable and active Ni-based core−shell catalyst. Furthermore, it offers novel insights into the functionalities of non-reducible spinel overlayers in the DRM process.
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Frontiers of Chemical Science and Engineering
·
2025
·Vol. 19
·期 10
·1-10
·
IF 4.5
Wang Lu,Li Zhiqiang,He Yangdong,Huang Chenzhi,Chen Shijin,Zhou Xianyun,Fan Xiaosong,Xie Wenjing,Wang Xuerui
Membrane gas separation is an energy-efficient approach to extract helium from natural gas. However, the limited separation performance shown as Robeson’s upper bound has hindered the techno-economic feasibility. This study introduces an advanced copolyimide membrane engineered for He extraction from natural gas. The membranes were facilely achieved by dip-coating the α -alumina substrates in the copolyimide solution followed by in situ thermal rearrangement. In addition to the rigid 5-amino-2-(4-aminobenzene)benzimidazole segments, the active ortho-hydroxyl groups were converted to benzoxazole rings, contributing to extra micropores. The membrane showed an improved mixture selectivity of 120 and He permeance of 23.5 GPU, far surpassing the performance of benchmark membranes for helium separation over CH 4 . The membrane also demonstrated long-term stability as evidenced by the continuous operation over 250 h. Additionally, the membrane exhibited resistance to impurities such as CO 2 and C 2 H 6 , enduring the asymmetric membranes promising for practical helium extraction from natural gas.
研究领域:
材料科学
·
化学工程
·
气体分离技术
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高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Jia Li,Ge Gao,Yang Liu,Yang Li,Zhi Liu
Stimulating photocatalytic activity of layered double hydroxides (LDHs) have been being as a research hotspot in photocatalysis . Quantum dots doping is a well acknowledged strategy to utilize their photoelectric superiorities to overcome the intrinsic defects of pristine LDHs. In this work, waste biomass-derived carbon quantum dots (B-CQDs)-interspersed CoAl-LDH photocatalysts (B/CALs) are successfully prepared by means of a simple hydrothermal method from green and renewable points of view. The introduction of B-CQDs significantly broadens the light absorption range and capacity of CoAl-LDH. As the terminal electron acceptor , the highly-dispersed B-CQDs can effectively prolong the lifetime of photogenerated charge carriers and promote the separation of photogenerated electron-hole pairs. No assistance from any sacrificial agent , the optimal sample of B/CAL-2 exhibits significantly enhanced photoreduction activity of CO 2 -to-CO and CH 4 , 6.4- and 7.5-fold higher than those of the pristine CoAl-LDH, respectively, and also surpassing many reported high-level LDHs counterparts. Such an uncomplicated case guides a green and feasible route to modify semiconductor materials with renewable biomass, which is expected to be applied to others for enhanced photocatalytic activity.
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高影响因子
FUEL
·
2022
·
IF 8.035
Chengming Huang,Yiming Zhang,Dingmei Han,Binbin He,Xinyu Sun,Meiyu Liu,Yi Mei,Yun Zu
Ni-based catalysts using siliceous materials as the supports have suffered from two challenging issues of sintering and carbon deposition for dry reforming of methane (DRM), resulted from a weak metal-support interaction. Given these, a novel metal–acid bifunctional Ni@S-1 zeolite catalyst is tailored from the evolution of hydroxylated nickel phyllosilicates that are formed by subtly controlling the coordination environments of Ni precursor complexes in the silicalite-1 (S-1) zeolite. The developed Ni 0.44 @S-1 catalyst renders almost equivalent CH 4 and CO 2 conversions (85.1 % and 88.7 %), high H 2 /CO molar ratio (about 1) and superb long-term stability during 100 h with no activity loss at 750 °C with a WHSV of 100 L·g cat −1 ·h −1 , outperforming other control catalysts under investigation. Such superior catalytic behavior benefits from the synergy between highly uniform Ni nanoparticles (3–5 nm) confined in the micropores of zeolite and substantially formed Lewis acid sites due to coordinatively unsaturated Ni 2+ sites located at the reduced 2:1 nickel phyllosilicate, as revealed by detailed characterizations. Meanwhile, it further discloses that a benign balance between formation and elimination of “process carbon” species is responsible for improving the carbon resistance of catalyst during the DRM reaction. The present design broadens a new insight for the development of new Ni-based catalysts with simultaneous coking- and sintering-resistant for the DRM application.
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Materials Today Communications
·
2022
·
IF 3.662
Shaocan Dong,Weiqiu Huang,Xufei Li,Xinya Wang,Baoyou Yan,Zhen Zhang,Jing Zhong
In response to global climate change, most countries have set carbon reduction targets. Mixed matrix membranes (MMMs), which combine the characteristics of inorganic nanofillers and organic matrices, have received wide attentions because of their good permeability and selective performance for the separation of CO 2 from industrial waste gases. However, the poor dispersion, compatibility and interfacial defects often lead to poor gas separation performance. In this paper, according to the dissolution-diffusion and Lewis acid-base theories, inorganic filler of amino-functionalized Bentonite (APTES-Bentonite) with -NH 2 was firstly synthesized to improve the affinity of CO 2 . Then, the dual-functionalized MMMs of APTES-Bentonite/PVDF (A-B/P MMMs) was prepared and adopted for the separation of CO 2 /CH 4 and CO 2 /N 2 , showing the increase of 87.76% and 75.31% compared to the pristine PVDF membrane, respectively. These excellent performances were attributed to the synergistic effect of APTES-Bentonite with -NH 2 groups and PVDF with -F groups, which provide a dual-functional transport pathway for CO 2 molecules due to the interactions of host-guest. Overall, the customized A-B/P MMMs offer superior CO 2 separation performance, which provides some valuable references for large-scale CO 2 capture studies.
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