ACS Applied Materials & Interfaces
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2024
·
IF 8.3
Yuntao Qi,Bin Zhang,Dengrong Xue,Hui Zhang,Xiaoning Liu,Zhi Liu,Shichao Zhao,Zhuo Li,Fanchun Meng,Yong Qin
The catalytic conversion of CO2 to CO through hydrogenation has emerged as a promising strategy for CO2 utilization, given that CO serves as a valuable C1 platform compound for synthesizing liquid fuels and chemicals. However, the predominant formation of CH4 via deep hydrogenation over Ru-based catalysts poses challenges in achieving selective CO production. High reaction temperatures often lead to catalyst deactivation and changes in selectivity due to dynamic metal evolution or agglomeration, even with a classic strong metal–support interaction. Herein, we have developed a FeOx/Ru/Rutile multilayer epitaxial structure by depositing a FeOx layer onto the epitaxially grown RuO2 nanolayers on the surface of rutile nanoparticles. This multilayer epitaxial structure transformed into a structure in which Ru nanoparticles were decorated with FeOx layers with ultrastable strong metal-support interaction (SMSI). Subsequently, the FeOx decoration on Ru nanoparticles effectively shifted the dominant product from CH4 to 95% CO during CO2 hydrogenation. Remarkably, this catalyst exhibits exceptional stability and can be operated stably at 550 °C for a long time without apparent deactivation. Compared with the dynamic changes observed in supported Ru nanoparticles, the interaction between Ru and FeOx maintains their electronic states at different reaction temperatures. Furthermore, this Ru–FeOx interaction inhibits H2 activation capability, CO adsorption, and subsequent hydrogenation of CO. The transformation strategy employed here, which utilizes initial multilayer epitaxial structures, can be applied to construct SMSI to enhance metal catalysts’ catalytic performance.
研究领域:
催化
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材料科学
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化学工程
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环境科学
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DOI
PubMed
高影响因子
ADVANCED ENGINEERING MATERIALS
·
2023
·Vol. 25
·期 22
·2301062
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IF 3.6
Binxia Yuan,Hong Qian,Lan Cao,Rui Zhu,Weiling Luan
Herein, H + in oxalic acid is used instead of Na + to obtain titanate nanosheets through P200 hydrolysis, which further curls to form a multilayer TiO 2 nanotubes (NTs) structure. Then, Cu 2 O quantum dots (QDs) are successfully loaded on TiO 2 NTs via a hydrothermal method using fructose as a reducing agent. The optical, impedance, and photocurrent tests indicate that the composite structure improves its optoelectronic performance. The photocatalytic H 2 production and CO 2 reduction efficiency of Cu 2 O QDs/TiO 2 NTs are lower than those of TiO 2 NTs. However, the molar ratio of CH 4 to CO produced by CO 2 reduction of Cu 2 O QDs/TiO 2 NTs composite catalyst is greater than that of pure TiO 2 NTs. The CH 4 production accounts for 97%, indicating that the composite catalyst has a high CH 4 selectivity. The experimental and density functional theory calculation results prove that the Z-scheme heterojunction accelerates the separation and transfer of photogenerated carriers, and broadens the absorption range of visible light.
研究领域:
材料科学
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纳米技术
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环境科学
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化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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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 .
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
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产品关联
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Yingying Cheng,Yuanye Zhuang,Shiyang Bai,Meng Ge,Jihong Sun,Jingjing Sun,Xufeng Gong
The removal of CO2 from biogas is critically important for environmental protection and energy applications yet remains technically challenging in the chemical industry. In this work, novel composite adsorbents featuring ZIF-8 uniformly dispersed on randomly oriented clinoptilolite lamellae (LCP) were designed and fabricated through a straightforward composite method. The synthesis sequentially incorporated metal precursors into LCP via ion exchange and salt addition and then introduced organic ligands to generate ZIF-8. Comprehensive characterizations, including XRD, FT-IR, N2 adsorption–desorption isotherms, SEM, and TG analyses, confirmed the physicochemical properties and structural features of the composites. The synthesized Zn-LCP/ZIF-8 materials exhibited exceptional CO2/CH4 separation performance, demonstrating ultralow CH4 adsorption capacity (<0.1 mmol/g) coupled with superior CO2/CH4 selectivity (≈28). Complementary molecular simulations using Material Studio software provided mechanistic insights into the adsorption and separation behavior, which further confirmed the superiority of the composite structure in CO2/CH4 separation. These results establish an effective strategy for biogas purification, while offering new perspectives for enhancing the CO2/CH4 adsorption selectivity.
研究领域:
环境科学
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能源技术
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材料科学
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化学工程
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吸附
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhai Jianxin,Xia Zhanghui,Zhou Baowen,Wu Haihong,Xue Teng,Chen Xiao,Jiao Jiapeng,Jia Shuaiqiang,He Mingyuan,Han Buxing
Upcycling of CO 2 into fuels by virtually unlimited solar energy provides an ultimate solution for addressing the substantial challenges of energy crisis and climate change. In this work, we report an efficient nanostructured Ru/MnO x catalyst composed of well-defined Ru/MnO/Mn 3 O 4 for photo-thermal catalytic CO 2 hydrogenation to CH 4 , which is the result of a combination of external heating and irradiation. Remarkably, under relatively mild conditions of 200 °C, a considerable CH 4 production rate of 166.7 mmol g −1 h −1 was achieved with a superior selectivity of 99.5% at CO 2 conversion of 66.8%. The correlative spectroscopic and theoretical investigations suggest that the yield of CH 4 is enhanced by coordinating photon energy with thermal energy to reduce the activation energy of reaction and promote formation of key intermediate COOH* species over the catalyst. This work opens up a new strategy for CO 2 hydrogenation toward CH 4 .
研究领域:
化学
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材料科学
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环境科学
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能源科学
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产品关联
DOI
PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Shenglong Wang,Jian Xu,Shuanshi Fan,Yanhong Wang,Xuemei Lang,Chi Yu
Clathrate hydrates is an ideal host for natural gas, by entrapping CH 4 molecules in cage-like structures composed of hydrogen-bonded water molecules, natural gas can be stored in solid form with high density. However, the suppression of hydrate dissociation under moderate thermodynamic conditions is still challenging. In this study, to increase the preservation stability of CH 4 hydrate at atmospheric pressure, a new surface-treatment method was proposed by coating CH 4 hydrate with CP-CH 4 hydrate. CH 4 hydrate pellets formed from ice powder or 0.03 wt% Sodium dodecyl sulfate (SDS) solution were mechanically pressurized with CP to form hydrate pellets. The presence of CP-CH 4 hydrate layer on the sample surface was confirmed by Raman spectroscopy, and the hydrate pellet was successfully preserved under superheated conditions, i.e., 0.1 MPa − 0.3 MPa, 279 K − 284 K with a storage volume density up to ~146 V CH4 (STP)/ V water , and the accumulated CH 4 loss was less than 0.3 mol% for hydrate pellet formed from ice powder, and 3 mol% for hydrate pellets formed from SDS solution for at least 8 h.
研究领域:
化学工程
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能源科学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 8
·2864-2872
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IF 6.119
Xiaoli Li,Yuan Tang,Yue Jiang,Manman Mu,Xiaohong Yin
A series of composites composed of Bi4O5Br2 and Fe-MIL were successfully fabricated for mimicking sunlight-driven photocatalytic reduction of CO2. Herein, Bi4O5Br2, as a modulator of solid acids, could turn NH2-MIL-101(Fe) into NH2-MIL-88B(Fe) completely at 0.07 wt% catalytic loading, where further addition could construct the corresponding composites of Bi4O5Br2 and NH2-MIL-88B(Fe). The highest activity in the photocatalytic reduction of CO2 was achieved at 7.96 μmol g−1 h−1 of CH4 at 3.28 wt% of Bi4O5Br2. Besides, this catalyst possessed high photostability during the recycling experiments and the mechanism of this process was thoroughly explored. This study provides a novel strategy employing solid acid modulators for regulating the structure and morphology of MOFs showing high activity and stability in the photocatalytic reduction of CO2 to CH4.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
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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.
研究领域:
材料科学
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催化
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环境化学
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光化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Tong Li,Xiaoxia Jia,Hui Chen,Zeyu Chang,Libo Li,Yong Wang,Jinping Li
Adsorption separation technology using adsorbents is promising as an alternative to the energy-demanding cryogenic distillation of natural gas (CH4/N2) separation. Although a few adsorbents, such as metal–organic frameworks (MOFs), with high performance for CH4/N2 separation, have been reported, it is still challenging to target the desired adsorbents for the actual CH4/N2 separation under humid conditions because the adsorption capacity and selectivity of the adsorbents might be mainly dampened by water vapor. Except for the high CH4 uptake and CH4/N2 selectivity, the adsorption material should simultaneously have excellent stability against moisture and relatively low-water absorption affinity. Here, we tuned the ligands and metal sites of reticular MOFs, Zn-benzene-1,4-dicarboxylic acid–1,4-diazabicyclo[2.2.2]octane (Zn-BDC–DABCO) (DMOF), affording a series of isostructural MOFs (DMOF-N, DMOF-A1, DMOF-A2, and DMOF-A3). Because of the finely engineered pore size and introduced aromatic rings in the functional DMOF, gas sorption results reveal that the materials show improved performance with a benchmark CH4 uptake of 37 cm3/g and a high CH4/N2 adsorption selectivity of 7.2 for DMOF-A2 at 298 K and 1.0 bar. Moisture stability experiments show that DMOF-A2 is a robust MOF with low water vapor capacity even at ∼40% relative humidity (RH) because of the presence of more hydrophobic aromatic rings. Breakthrough experiments verify the excellent CH4/N2 separation performances of DMOF-A2 under high humidity.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2023
·Vol. 58
·期 5
·2140-2155
·
IF 4.5
Zhang Yeguang,Li Yingchao,Liu Wenxin,Li Feihu,Zhan Zili
CH 4 sensors based on metal oxide semiconductors (MOS) provide high sensitivity and fast response, but the sensitivity will be lost when they are poisoned by silicone. Therefore, there is an urgent need to address the poisoning deactivation of MOS gas sensors caused by silicone. Here, the unique strategy of coating a reactive anti-poisoning material onto the surface of the sensing material is proposed to effectively improve the anti-poisoning ability without degrading the gas sensing performance. As an experimental verification, SnO 2 /α-Al 2 O 3 is designed as the anti-poisoning layer and SnO 2 loaded with precious metals (Pt and Pd) as the sensing layer. Owing to the protection of the anti-poisoning layer, the response ( R a / R g = 24.69) and the response/recovery time (1/24 s) of the sensor to CH 4 remained undiminished at 364 °C after being poisoned under an air/hexamethyldisiloxane (HMDSO) (10 ppm) environment for 40 min, which meets the requirements of the Chinese National Standard (GB 15322.2-2019). The mechanism analysis shows that HMDSO can be decomposed with the adsorbed oxygen on the surface of SnO 2 in the anti-poisoning layer, and CH 4 can diffuse into the sensing layer to be detected. The unique anti-poisoning strategies can provide a promising insight for improving the poisoning tolerance of MOS gas sensors. Graphical abstract
研究领域:
材料科学
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化学工程
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传感技术
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产品关联
DOI
高影响因子
Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-15
·
IF 26.6
Li Minhan,Zhang Fangzhou,Kuang Min,Ma Yuanyuan,Liao Ting,Sun Ziqi,Luo Wei,Jiang Wan,Yang Jianping
Electrochemical reduction of CO 2 into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO 2 capture and utilization, resulting from their high catalytic activity and selectivity. The mobility and accessibility of active sites in Cu-based catalysts significantly hinder the development of efficient Cu-based catalysts for CO 2 electrochemical reduction reaction (CO 2 RR). Herein, a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride (g-C 3 N 4 ) as the active sites for CO 2 -to-CH 4 conversion in CO 2 RR. By regulating the coordination and density of Cu sites in g-C 3 N 4 , an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH 4 Faraday efficiency of 49.04% and produces the products with a high CH 4 /C 2 H 4 ratio over 9. This work provides the first experimental study on g-C 3 N 4 -supported single Cu atom catalyst for efficient CH 4 production from CO 2 RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO 2 RR by engineering Cu active sites in 2D materials with porous crystal structures.
研究领域:
化学
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材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Jinqiang Sun,Jing Zhang,Xiaoqian Peng,Xu Zhang,Zhipeng Yuan,Xiaochan Liu,Sijia Liu,Xinfu Zhao,Shimo Yu,Xibin Yi
Biomass aerogel is attractive in various applications due to their renewable, biodegradable and eco-friendly advantages. Herein, a novel beta molecular sieve/carboxymethyl cellulose/polyvinyl alcohol composite aerogel (beta/CP) is prepared by direct mixing and directional freeze-drying as an efficient gas adsorbent with hierarchical porosity. The beta molecular sieve is uniformly dispersed in the three-dimensional skeleton of the aerogel. By adjusting the loading mass of the beta molecular sieve to constitute a reasonable porosity and pore size distribution , the synergistic effect between pore structures of different scales improves the adsorption performance. The experiment results of beta/CP-4 show that the CH 4 adsorption capacity can reach 60.33 cm 3 /g at 298 K and 100 bar, which is almost the same as that of the pure beta molecular sieve (62.09 cm 3 /g). The strong interaction between the aerogel and it prevents the molecular sieve agglomeration, improves the pore utilization, and also reduces the cost of using molecular sieve adsorbent. The above results indicate that the composite has good potential for application in the field of CH 4 storage.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）