Journal of Physical Chemistry C
·
2023
·
IF 3.7
Zhan-Kuo Guo,Han-Qing Chen,Hui-Lin Jiang,Bao-Xia Dong,Yun-Lei Teng
Storing and hydrogenating CO2 to CH4 is an efficient solution to alleviate the greenhouse effect and energy shortage. This work demonstrated that the CaO-captured CO2 could be selectively converted to CH4 by Ni- and hydrogen-assisted calcium looping (CaL) processes in a batch reactor. The Ni/CaO composite was first synthesized in one step at room temperature by calcium-induced hydrogenation of Ni-mixed calcium carbonate without the use of any solvent and CO2 emission. The CO2 capture properties over the Ni/CaO composite and the methanation properties of the Ni/CaCO3 composite produced after CO2 capture were then studied in a batch reactor. It was proved that the CO2 capture properties of CaO can be improved, the CaO recovering temperature can be significantly lowered, and valuable CH4 can be selectively produced by Ni- and hydrogen-assisted calcium looping processes at moderate/high temperature. The 68.58% methane yield and 100% methane selectivity were achieved under relatively mild conditions. After five Ni- and hydrogen-assisted CaL processes, the methane yield still reaches 45%. This study offers a novel energy-saving CaL process, which can be utilized for facile and selective conversion of the CaO-captured CO2 to CH4.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Zengqi Liu,Shuting Zhang,Yingying Liu,Qiang Sun,Zhen Xu,Aixian Liu,Yiwei Wang,Xuqiang Guo
The accurate prediction of thermodynamic equilibrium hydrate formation pressure ( P eq ) is crucial to the industrial application of hydrate-based gas separation. This study evaluated P eq of CH 4 -CO 2 gas mixtures with different TBAB solutions at different temperatures. Unlike previously reported models, the proposed model accounted for the effects of interaction of multiple solutes and the deformation of dodecahedral (D)-cages on P eq , thereby minimizing deviations in predictions. The effects of the interaction of multiple solutes on P eq can be attributed to gas dissolution and the presence of electrolytes. For accurate prediction, the proposed model incorporated the aforementioned effects based on the electrolyte-cubic plus association equation of state and the parameters for interaction among guest molecules in cages Furthermore, the proposed model can quantitatively describe the effects of gas dissolution, the presence of electrolytes and deformation of D-cages on the P eq values for corresponding systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Lingxiang Huang,Yue Ma,Mufan Niu,Shenyong Ren,Qiaoxia Guo,Chunming Xu,Baojian Shen
Dry reforming reaction of greenhouse gas CH 4 and CO 2 was studied over Ni-Fe bimetallic catalyst, in which the composite support of C12A7-O 2- in MCM-41 was used. The isotope 13 CH 4 /D 2 O tracing experiment showed CO mainly comes from 13 CHx oxidation reaction and DH comes from CHx and D 2 O reaction, exhibiting lattice oxygen promotes CH X oxidation and water accelerate methane conversion. XPS and TPSR-MS studies exhibited the existence of lattice oxygen in catalysts produces a little H 2 O to facilitate a lower starting point at the reaction temperature. On-line MS investigation found that the trace water addition in the system accelerated the adsorption of CO 2 on support and promoted methane dissociation, the H 2 signal appears later than CO, indicating the oxidation reaction of CHx occurs after the dissociation of CO 2 . Besides, TG analysis tells us the H 2 O may consume Cα on the catalyst in time during the reaction process to remove carbon deposition.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongli Yang,Huilin Hou,Man Yang,Zhongli Zhu,Hui Fu,Dongdong Zhang,Yong Luo,Weiyou Yang
The selective photoreduction of CO 2 into hydrocarbon fuels, such as CH 4 , is highly desirable for sustainable energy but remains a significant challenge due to slow proton-electron transfer processes and competing intermediates. Herein, a novel NiO/MgAl-LDH (NMA-x, LDH represents layered double hydroxide) step-scheme (S-scheme) heterojunction has been engineered via in-situ anchoring MgAl-LDH nanoplates on metal–organic frameworks (MOFs) derived NiO microrods, which improves the CO 2 adsorption capability and specific surface area of NiO. The steered internal electric field in the p-n heterointerface promotes charge separation and attracts a high electron density center on the catalyst surface to favor CH 4 production. Meanwhile, S-scheme photogenerated charge transfer mechanism is proposed by in-situ X-ray photoelectron spectroscopy (XPS), in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectra and density functional theory (DFT) calculation. In this process, photogenerated electrons are transferred from the conduction band (CB) of MgAl-LDH to the valence band (VB) of NiO, facilitating the CHO* species serve as the critical intermediate for producing CH 4 through desired photocatalytic CO 2 reduction. Using pure water as a proton source, the NMA-2 catalyst achieved a high CH 4 selectivity of 91.2% and a yield of 8.98 μmol∙g −1 ∙h −1 , representing significant potential for practical applications. This catalyst outperformed pristine and revitalized NiO by 4.23 and 2.07 times, respectively.
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ACS Sustainable Chemistry & Engineering
·
2020
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IF 7.632
Yu Chen,Yanfei Zhao,Bo Yu,Yunyan Wu,Xiaoxiao Yu,Shien Guo,Buxing Han,Zhimin Liu
A novel four-site ionic liquid (IL) was designed via the neutralization of citrazinic acid with tetrabutylphosphonium hydroxide, which had the highest CO2 absorption capacity of 3.26 mol per molar IL under ambient conditions to date. More importantly, it was found that the IL–CO2 complex displayed visible light absorption because of the delocalization effect in the conjugated anion complex, and it could promote the photoreduction of CO2 over anatase TiO2 under visible light irradiation, producing CH4 as the sole carbonaceous product with a rate of 3.52 μmol g–1 h–1 and a selectivity of >96%. The mechanism investigation indicated that the IL absorbed CO2 to form the IL–CO2 complex showing visible light absorption, which served as a photosensitizer to promote the photoreduction of CO2 over TiO2 under visible light irradiation. This work opens a new way to enhance visible light-driven photoreduction of CO2, which may have promising application.
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CHEMOSPHERE
·
2020
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IF 5.778
Jiuhu Zhao,Gaige Zhang,Jiansheng He,Zhengzhong Wen,Zhi Li,Tingkun Gu,Ran Ding,Yongji Zhu,Rongshu Zhu
In/H-Beta catalyst was prepared by optimizing the support, concentration of ion exchange liquid and calcination temperature to investigate the effects of synthesis conditions on catalytic activity of selective catalytic reduction of NO x with CH 4 . The results showed that the In/H-Beta catalyst exhibited the superior activity when concentration of exchange liquid was 0.033 M and calcination temperature was 500 °C, the NO x removal ratio could reach 97.6%. In addition, reaction conditions could affect the catalytic performance. When O 2 concentration was 10%, CH 4 :NO ratio was no less than one, space velocity was lower than 23600 h −1 and NO initial concentration was no more than 700 ppm, In/H-Beta could exhibit superior catalytic activity. Moreover, the catalytic performances of In/H-Beta catalysts were discussed after enduring H 2 O or/and SO 2 . This novel strategy could open the door for selective catalytic reduction of NO x with CH 4 .
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CHINESE JOURNAL OF CATALYSIS
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2016
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IF 2.628
Qi Sun,Xianglan Xu,Honggen Peng,Xiuzhong Fang,Wenming Liu,Jiawei Ying,Fan Yu,Xiang Wang
A series of SnO 2 -based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M (M = Mn, Zr, Ti and Pb) molar ratio of 9/1 were prepared by a co-precipitation method and used for CH 4 and CO oxidation . The Mn 3+ , Zr 4+ , Ti 4+ and Pb 4+ cations are incorporated into the lattice of tetragonal rutile SnO 2 to form a solid solution structure. As a consequence, the surface area and thermal stability of the catalysts are improved. Moreover, the oxygen species of the modified catalysts become easier to be reduced. Therefore, the oxidation activity over the catalysts was improved, except for the one modified by Pb oxide. Manganese oxide demonstrates the best promotional effects for SnO 2 . Using an X-ray diffraction extrapolation method, the lattice capacity of SnO 2 for Mn 2 O 3 was 0.135 g Mn 2 O 3 /g SnO 2 , which indicates that to form stable solid solution, only 21% Sn 4+ cations in the lattice can be maximally replaced by Mn 3+ . If the amount of Mn 3+ cations is over the capacity, Mn 2 O 3 will be formed, which is not favorable for the activity of the catalysts. The Sn rich samples with only Sn-Mn solid solution phase show higher activity than the ones with excess Mn 2 O 3 species.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yuan-Sheng Cheng,Xiao-Wan Xiong,Xue-Feng Cao,Min Ling,Yuwen Cheng,Fang-Hui Wu,Qiyan Xu,Xian-Wen Wei
Due to the complex series of elementary steps involved, achieving deep photoreduction of CO2 to multielectron products such as CH4 remains a challenging task. Therefore, it is crucial to strategically design catalysts that facilitate the controlled formation of the crucial intermediates and provide precise control over the reaction pathway. Herein, we present a pioneering approach by employing polyhydroxy fullerene (PHF) molecules to modify the surface of Ni(OH)2, creating stable and effective synergistic sites to enhance the formation of CH4 from CO2 under light irradiation. As a result, the optimized PHF-modified Ni(OH)2 cocatalyst achieves a CH4 production rate of 455 μmol g–1 h–1, with an electron-based selectivity of approximately 60%. The combination of in situ characterizations and theoretical calculations reveals that the hydroxyl species on the surface of PHF can participate in stabilizing crucial intermediates and facilitating water activation, thereby altering the reaction pathway to form CH4 instead of CO. This study provides a novel approach to regulating the selectivity of photocatalytic CO2 reduction by exploring molecular surface modification through interfacing with functionalized carbon clusters.
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高影响因子
MOLECULES
·
2024
·Vol. 29
·期 16
·3747
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IF 4.2
Guanyu Chen,Weixin Zhang,Rongshu Zhu,Yanpeng Chen,Minghu Zhao,Mei Hong
Zeolite-based catalysts efficiently catalyze the selective catalytic reduction of NOxwith methane (CH4-SCR) for the environmentally friendly removal of nitrogen oxides, but suffer severe deactivation in high-temperature SO2- and H2O-containing flue gas. In this work, SSZ-39 zeolite (AEI topology) with high hydrothermal stability is reported for preparing CH4-SCR catalysts. Mild acid leaching with oxalic acid (OA) not only modulates the Si/Al ratio of commercial SSZ-39 to a suitable value, but also removes some extra-framework Al atoms, introducing a small number of mesopores into the zeolite that alleviate diffusion limitation. Additional Co3O4modification during indium exchange further enhances the catalytic activity of the resulting In-Co3O4/H-SSZ-39(OA). The optimized sample exhibits remarkable performance in CH4-SCR under a gas hourly space velocity (GHSV) of 24,000 h−1and in the presence of 5 vol% H2O. Even under harsh SO2- and H2O-containing high-temperature conditions, it shows satisfactory stability. Catalysts containing Co3O4components demonstrate much higher CH4conversion. The strong mutual interaction between Co3O4and Brønsted acid sites, confirmed by the temperature-programmed desorption of NO (NO-TPD), enables more stable NxOyspecies to be retained in In-Co3O4/H-SSZ-39(OA) to supply further reactions at high temperatures.
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Surfaces and Interfaces
·
2025
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IF 6.3
Ming Liu,Nan Sun,Ruohan Xu,Tallat Munir,Shiyang Bai,Jihong Sun
The surfactant involvement in hydrothermal synthesis system of clinoptilolite (CP) is an effective strategy for regulating self-assemble of the aluminosilicate species. Herein, using cetyltrimethylammonium bromide (CTAB) as surfactant, the CTAB-assisted influences on nucleation behavior of CP were demonstrated via various characterizations. Especially, small angle X-ray scattering patterns were used to investigate the fractal structural evolutions of aluminosilicate species in their sol-gel phase. The results indicated that the primary building structural units with 8- and 10-membered rings appeared in the early induced stage gradually aggregated into the worm-liked particles with the prolonged crystallization time. Among them, the nucleation process was initiated by reorganization via the solution-mediated transport and thereafter appeared the pseudo-layered structures with the core (aluminosilicate species)-shell (CTAB) features at the liquid-solid interfaces. The irregulated lamellas with the heulandite structures increased in size of around 70 nm until reaching the maximum of 90 nm, then followed the occurrences of the re-dissolving and repaid growth. Especially, the lamellar nuclei growth showed the transformations from loose mass fractals to dense surface fractals with the extensions of the induced time. In which, the interfacial solvation layer thickness increased from 1.04 to 2.87 nm for CTAB-assisted CP, thicker than that (0.63–2.08 nm) for pure-CP. These demonstrations suggested that the additive CTAB in the induced stage inhibited the agglomeration of the aluminosilicate species and following growth of the crystal nuclei via the solvated attachments pathway. Finally, using the irregulated particle as an adsorbent, the CO 2 adsorption and CO 2 /CH 4 selectivity were preliminarily explored.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jun Wu,Shangzhi Song,Lei Wang,Ruoping Li,Jiaqi Wen,Yanan Guo,Jing Ding,Danhua Mei,Hui Wan,Guofeng Guan
Non-thermal plasma is one of the most promising technologies for converting CH 4 and CO 2 into value-add chemicals under ambient pressure and room temperature. However, the challenge still lies in exploring efficient catalysts and deeply clarifying the relationship between the structure of catalyst and its catalytic performance. Herein, the Cu single-atom (Cu-N 4 coordination structure) anchored in carbon nitride catalyst (CuSA-CN) is prepared by coordination pyrolysis, which not only efficiently enhances the plasma-catalytic conversion of CH 4 and CO 2 with high selectivity of CH 3 COOH, but exhibits a good stability. Characterizations and DFT calculations reveal that the combination of the excellent physical discharge properties and the charge transfer between Cu single atom and carrier is beneficial for activating of CH 4 and CO 2 . Meanwhile, Cu single-atoms reduce the energy barriers of CH 4 dissociation and C–C coupling, thereby promoting CH 3 COOH generation. This work provides new insights into designing single-atom catalysts for application in non-thermal plasma catalytic reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Bo Feng,Tingman Zhao,Jiada Du,Jiyuan Hu,Yun Shi,Jingkai Zhao,Jianmeng Chen
Methane selective catalytic reduction (CH 4 -SCR) technology has shown promise for controlling NO x emissions from natural gas generator sets. This study presents a highly efficient Ce 30 In 15 /HBEA catalyst featuring dual active sites, Al-O – (InO + )-Si site for CH 4 activation and ceria oxygen vacancy (Ce 3+ -□) site for NO x activation. However, the CH 4 -SCR activity of this catalyst decreased in the presence of H 2 O, SO 2 , C 3 H 6 , and CO 2 . The inhibitory effects on CH 4 -SCR activity followed by the sequence: H 2 O > SO 2 > C 3 H 6 > CO 2 . In particular, H 2 O combined with Al-O – (InO + )-Si to form inactive In(OH) 3-z z+ species and occupied Ce 3+ -□, preventing Ce 4+ -NO 3 – /NO 2 – formation. In/Ce sulfate formation via the reaction between SO 2 and In/Ce active sites hindered CH 4 and NO x adsorption and activation. The formed carbon deposits covered the active sites on the catalyst surface due to incomplete C 3 H 6 oxidation . In comparison, the dual active sites were almost unaffected by CO 2 . Overall, this study provides a basis for the rational design of novel catalysts for CH 4 -SCR.
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