APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Xinxin Zhang,Kang Hu,Xuliang Zhang,Wajid Ali,Zhijun Li,Yang Qu,Hao Wang,Qingyang Zhang,Liqiang Jing
In this work, an in-situ way has been developed to achieve the co-modification of highly-dispersed Mn and Cu oxides to g-C 3 N 4 nanosheets for efficient CO 2 reduction. The Mn & Cu amount-optimized nanosheets exhibit the improved photocatalytic activity for CO 2 reduction to CO and CH 4 both by 3 times compared with the generally-bulk g-C 3 N 4 , mainly attributed to the nanosheet structure and to the roles of modified Mn and Cu oxides. Based on the transient-state surface photovoltage responses, transient-state photoluminescence spectra, and electrochemical measurements, it is confirmed that the modified Mn and Cu oxides could respectively capture the photogenerated holes and electrons, and provide the catalytic functions for water oxidation and CO 2 reduction. Remarkably, the simultaneous introduction of Mn and Cu oxides shows an obvious synergistic effect on the improvement of photocatalytic activity for CO 2 reduction. This work provides a feasible way to synthesize high-activity g-C 3 N 4 -based photocatalysts for energy production.
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REACTIVE & FUNCTIONAL POLYMERS
·
2019
·
IF 3.074
Xing Yang,Yayun Zheng,Lan Wang,Qingping Guo,Haiquan Shan,Zongxiang Xu,Jujie Luo
This work involves the preparation and characterization of poly(styrene-b-isoprene-b-styrene)-poly(dimethylsiloxane- co -methylhydrosiloxane) (SIS-c-PDMS-co-PMHS) crosslinked membranes towards CH 4 /N 2 separation. SIS-c-PDMS-co-PMHS was synthesized via a simple hydrosilylation reaction with various PDMS-co-PMHS contents. The structure of crosslinked membranes was investigated by Fourier transform infrared spectroscopy , indicating the degree of hydrosilylation reaction. The morphology of sample membranes was observed in detail by means of Scanning Electron Microscope analysis . Thermodynamic stability and the crosslinked behavior of crosslinked membranes were explored by thermogravimetric analysis and Soxhlet extraction experiments. Furthermore, single gas (CH 4 , N 2 ) permeability was measured using the time-lag method. The CH 4 permeability of crosslinked membranes with 70 wt% PDMS-co-PMHS could reach 503 Barrer at 25 °C and 1 bar, which is significantly greater than that of SIS (25.9 Barrer), while the CH 4 /N 2 ideal selectivity hardly changed. Notably, CH 4 permeability further improved by 77.6% (893.4 Barrer) as the temperature increased to 55 °C. For the CH 4 /N 2 (50/50 vol%) mixed gas, the SIS-c-PDMS-co-PMHS-70 sample membrane exhibited ideal gas separation performance relative to that of the pure SIS membrane (CH 4 : 447.4 vs. 24.2 Barrer，N 2 : 188.1 vs. 9.46 Barrer).
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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Ziqiong Wang,Yan Wang,Wanting Li,Siyu Liu,Ling Zhang,Jiani Yang,Caixia Feng,Ruifeng Chong,Yanmei Zhou
Solar-light-driven reduction of CO 2 into renewable fuels has great potential in the production of sustainable energy, addressing the energy crisis and environmental problems simultaneously. However, it is a significant challenge to achieve high selectivity for the conversion of CO 2 into CH 4 , which is a type of fuel with a high calorific value. Herein, carbon quantum dots (CQDs) were integrated with an oxygen vacancy modified nickel-based metal organic frameworks (NiMOFs) to form the CQDs-X/NiMOF V series, which exhibited superior performance for CO 2 photoreduction into CH 4 compared with pure NiMOFs in the presence of hole scavengers under visible light irradiation. The highest yielding rate of CH 4 (1 mmol g −1 h −1 ) and selectivity (97.58 %) were obtained using a CQDs-25/NiMOF V catalyst. Most importantly, in diluted CO 2 atmosphere, the yield of CH 4 was almost unchanged and the selectivity of CH 4 over CQDs-25/NiMOF V was higher than that in pure CO 2 . The superior performance of CQDs-25/NiMOF V may be attributed to the following two factors: (i) both CQDs and oxygen vacancies facilitate the transmission of electrons to promote the eight-electron reaction producing CH 4 , and (ii) oxygen vacancies can act as the electron trap to capture the photogenerated electrons to react with adsorbed CO 2 on Ni 2+ . This study offers a valuable strategy for designing efficient photocatalysts to convert CO 2 into CH 4 with superior selectivity.
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APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Kai Li,Junqi Cai,Yue Tao,Yunhe Xing,Zuchao Zhu,Zhiqiang Lu,Xuming Zhang
The direct conversion of methane into the value-added chemical methanol using molecular oxygen was investigated via plasma catalysis under mild condition. An efficient synergistic effect between plasma and catalyst was achieved using an oxygen vacancy-rich ZnO/Al 2 O 3 catalyst. A high methanol selectivity of 48.5 % and a high synergy factor of 2.1 could be achieved simultaneously over ZnO/Al 2 O 3 R300 catalyst. The presence of oxygen vacancies played a crucial role in methanol formation. A close relationship between oxygen vacancy content and methanol selectivity was established. In situ DRIFT and optical emission spectra were employed to identify key intermediates, and a plausible reaction mechanism was proposed. The CH 3 and CH 3 O species were the key intermediates on the catalyst surface. The oxygen vacancy could efficiently adsorb the O radicals and accelerate the formation of CH 3 O species. This work offers insights into the rational engineering of efficient catalyst for plasma catalysis process.
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Carbon Capture Science & Technology
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2022
·
IF 0
Xinrui Wang,Shanshan Xu,Weiting Yang,Xiaolei Fan,Qinhe Pan,Huanhao Chen
This study presents an investigation of using Co doping strategy to improve the Ni on mesoporous SBA-15 catalyst for promoting catalytic dry reforming of methane (DRM) under non-thermal plasma (NTP) conditions. The work was conducted by following the conventional procedures including pre-/post-reaction characterisation of the relevant catalysts, comparative assessment of various scenarios under the NTP condition and longevity tests. However, we found that the performance enhancement of the NTP system was mainly due to the use of the catalytically inert SBA-15 packing, rather than the variation of metal species on it though the results suggest the possible surface reactions on the metal surfaces. Hence, under the NTP condition, the so-called DRM might be mistaken because (i) the production of H 2 and CO was likely due to the electron-impact dissociation of CO 2 /CH 4 in gas discharge and (ii) surface reactions on a DRM catalyst are rather insignificant. We then carefully analysed and reflected on the findings and proposed further research questions to be shared with the colleagues in the field of NTP catalysis.
研究领域:
化学工程
·
催化科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Yue Shen,Jielian Yang,Bing Chen,Chunyan Zhou,Liya Zhou,Binbin Luo,Qi Pang,Peican Chen,Xuetang Xu,Anxiang Guan
Developing efficient electrocatalysts capable of achieving effective electrochemical CO 2 -to-CH 4 conversion over a broad potential window remains a significant challenge in the field. Herein, we present a facile strategy for the synthesis of inverse CeO 2 /CuO catalysts through a hydrothermal approach, wherein CeO 2 nanodomains are supported on the surface of CuO. This catalyst exhibits exceptionally high CH 4 selectivity across the investigated voltage range, with a peak Faradaic efficiency of 63.6% and a corresponding partial current density of −472.9 mA cm −2 at −1.6 V vs. RHE, while the pure CuO catalyst without CeO 2 component was found to be active for electroreducing CO 2 to C 2+ products (C 2 H 4 ), as the adjacent Cu sites were beneficial for adsorbing multiple *CO intermediates and subsequent C C coupling. The incorporation of CeO 2 into Cu 1 Ce 9 -O x exerts a dual regulatory effect, synergistically suppressing C C coupling by reducing *CO coverage and optimizing *CO protonation kinetics for enhanced CH 4 selectivity. The presence of CeO 2 not only blocks the active sites of CuO for CO 2 -to-*CO intermediate conversion (thus lowering *CO coverage) but also facilitates water dissociation to generate abundant *H species, which subsequently migrate to Cu sites in Cu 1 Ce 9 -O x catalyst through the coherent interface between CuO and CeO 2 . These *H species subsequently facilitate the hydrogenation of *CO intermediates, ultimately resulting in CH 4 formation. Density functional theory (DFT) calculations demonstrate that CuCe-O x catalyst with strong H 2 O dissociation capability decreases the energy barrier for *CHO formation and favors *CO → *CHO conversion, thereby promoting CO 2 RR-to-CH 4 conversion. This work provides an effective strategy to enhance *H generation and the hydrogenation of *CO intermediates, thereby offering a feasible approach to improve CH 4 production efficiency in electrochemical CO 2 conversion. Compared with pristine CuO, CeO 2 nanodomains anchored on CuO surfaces redirect CO 2 electroreduction selectivity from C 2 H 4 to CH 4 . The presence of CeO 2 not only modulate *CO intermediate coverage but also accelerate H 2 O dissociation to produce abundant *H species, thereby promoting *CO protonation and boosting CH 4 formation with enhanced Faradaic efficiency. Download: Download high-res image (170KB) Download: Download full-size image
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FUEL
·
2025
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IF 7.5
Zhiwei Chu,Wenzhe Zhang,Wenhan Zhao,Duo Xu,Zirui He,Kuihua Han,Yingjie Li
H 2 and solid carbon are available through the CH 4 decomposition with Fe-based catalysts. Red mud is a solid waste containing lots of Fe 2 O 3 . In this work, the CeO 2 -doped solid waste-based catalyst pellets were prepared by the extrusion-spheronization method using red mud and calcium carbide slag for catalytic decomposition of CH 4 . The mass ratio of red mud to calcium carbide slag was 1:3. Regeneration of catalyst pellets with carbon deposits was performed by sieving separation and steam gasification. The effects of CeO 2 , catalyst pellet diameter, fluidization velocity, ratio and type of pore forming agent (bagasse, corn cob, horsetail pine, and walnut), ratio of binder (polyvinylpyrrolidone (PVP)), and pellet calcination duration on CH 4 decomposition and regeneration of catalyst pellets were studied in a fluidized bed reactor. The electrochemical performance of the Na-ion battery using the partial solid carbon materials from CH 4 decomposition as the anode materials was evaluated. The heat and mass transfer performance of catalyst pellets in fluidized state is enhanced. The initial CH 4 conversion is 88% in the first catalysis/regeneration cycle at 850 °C with the catalyst pellet diameter of 250–425 µm, calcination duration of 60 min, corn cob addition of 3 wt%, PVP addition of 2 wt% and fluidization velocity of 0.07 m/s. The CO 2 capture by CaO in catalyst pellets during gasification boosts the residual carbon deposits removal. The reversible sodium storage capacity of the Na-ion battery using solid carbon as the carbon-based anode material is 392.0 mAh/g. The CeO 2 -doped solid waste-based catalyst pellets are beneficial to the H 2 production, high-value utilization of solid carbon, and CO 2 capture via CH 4 decomposition and regeneration process.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 16
·11595-11606
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IF 2.993
Wu Keliang,Dong Xuejun,Zhu Junfang,Wu Pengcheng,Liu Chang,Wang Yixi,Wu Jianning,Hou Juan,Liu Zhiyong,Guo Xuhong
The nanostructured heterojunction photocatalysts are considered promising in photocatalytic reduction in the carbon dioxide. Herein, we demonstrate a simple sol–gel and hydrolysis process to design nanostructured TiO 2 /ZnO heterojunction, by using the biological template celery stalk. The nanostructured photocatalyst consists of anatase TiO 2 and wurtzite ZnO nanoparticles. A well-connected heterojunction, with uniformly distributed nanoparticles, on the pores and folds of celery stems, is obtained. The enhanced specific surface area of 55.5 m 2 /g is achieved. The crystal structure, morphology and surface composition are investigated by electron microscopy, X-ray photoelectron spectroscopy and X-ray diffraction. Furthermore, we demonstrate the photocatalytic performance of as-synthesized nanostructure TiO 2 /ZnO heterojunction. The photocatalytic yield, of CO 2 reduction into CH 4 , exhibits a five times increase, from 0.55 to 2.56 µmol h −1 g −1 , for the nanocomposite as compared to the pure TiO 2 . This enhanced performance corresponds to the efficient charge transfer and hindrance in the recombination of electron–hole pairs due to the optimum band positions of ZnO and TiO 2 . This study demonstrates the potential of using biotemplates to design efficient photocatalysts to convert CO 2 into useful solar fuels.
研究领域:
材料科学
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环境科学
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纳米技术
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光催化
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可持续能源
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2025
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IF 1.9
Sarmad Soomro,Zhenkun Sun,Dennis Y. Lu,Zhihao Zhou,Lin Li,Lunbo Duan
Catalyst deactivation due to carbon deposition and sintering poses a significant challenge to the efficient dry reforming of CH 4 and CO 2 into syngas, particularly at high Ni loadings. To tackle this difficulty, ordered mesoporous silicas with varied pore symmetries were employed as supports in this study to synthesize the Ni-based catalysts using hydrothermal treatment. The 10% Ni/MCM-41 catalyst exhibited the highest conversion rates for CO 2 (81%) and CH 4 (77%), with favourable H 2 /CO (0.92) ratios indicating efficient syngas production Higher Ni concentrations increase active sites and catalytic performance, they also increase carbon deposition, reducing catalyst durability. At lower Ni loadings (4% Ni), catalysts with a 3D pore structure showed improved activity and stability, effectively reducing carbon deposition. This study demonstrates that optimized mesopore symmetries and Ni loadings can enhance catalyst efficiency and durability for syngas production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qianqian Hu,Yuanzhi Li,Huamin Cao,Lei Ji,Jichun Wu,Mengqi Zhong
Using inexhaustible solar energy to drive efficient light-driven thermocatalytic CO 2 reduction by CH 4 (DRM) is an attractive approach that can synchronously reduce the greenhouse effect and convert solar energy into fuels. However, it is often limited by the intense light intensity required to produce high fuel production rates, and the catalyst deactivation due to severe carbon deposition generated from side reactions. Herein, a nanostructure of alumina-cluster-modified Ni nanoparticles supported on Al 2 O 3 nanorods (ACM-Ni/Al 2 O 3 ) was synthesized, displaying good catalytic performance under focused UV–vis-IR illumination. By light-driven thermocatalytic DRM on ACM-Ni/Al 2 O 3 at a reduced light intensity of 76.9 kW m −2 , the high fuel production rates of H 2 ( r H2, 65.7 mmol g −1 min −1 ) and CO ( r CO, 78.8 mmol g −1 min −1 ), as well as an efficient light-to-fuel efficiency ( η , 26.3 %) are achieved without additional heating. The r H2 and r CO of light-driven thermocatalysis are 2.9 and 1.9 times higher, respectively, compared to conventional thermocatalysis at the same temperature. We have discovered that high light-driven thermocatalytic activity originates from the photoactivation effect, significantly reducing the apparent activation energy and facilitating C* oxidation as a decisive step in DRM. ACM-Ni/Al 2 O 3 possesses excellent durability and exhibits an extremely low coking rate of 4.40 × 10 −3 g c g catalyst −1 h −1 , which is 26.8 times lower than that of the reference sample without Al 2 O 3 cluster modification (R-Ni/Al 2 O 3 ). This is owing to a decrease in activation energies (E a ) of C* oxidation and an increase in E a of C* polymerization by the surface modification of Ni nanoparticles with Al 2 O 3 clusters, effectively inhibiting carbon deposition.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Xing Yuan,Lingquan Meng,Chaohe Zheng,Haibo Zhao
Perovskites have been recognized as affordable substitutes for noble-metal catalysts for their tunable catalytic activity and thermal stability. Nevertheless, the highly demanding synthesis procedure still hinders the application of perovskites in catalytic combustion. In this work, a series of nanostructured SiTiO3 perovskites with B-site partial substitution by Co, Fe, Mn, Ni, and Cu are synthesized via flame spray pyrolysis in one step. The comprehensive characterizations on textural properties of nanostructured perovskites reveal that the flame-made perovskite nanoparticles all exhibit high crystal purity and large specific surface area (∼40 m2/g). Furthermore, the highest catalytic activity is achieved by SrTi0.5Co0.5O3 due to the formation of favorable oxygen vacancies, outstanding reducibility, and oxygen desorption capability. Additionally, the presence of 10 vol % water vapor during long-term testing indicates remarkable durability and water resistance. Finally, the CO oxidation and CH4 dehydrogenation on SrTiO3 incorporating Co atoms are more thermodynamically and kinetically favorable than those on other doped surfaces.
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