CATALYSIS COMMUNICATIONS
·
2022
·
IF 3.51
Baohuai Zhao,Baofang Jin,Xiaodong Wu,Duan Weng,Rui Ran
A series of Sm-Mn oxides (SmMnO 3 , SmMn 2 O 5 and Sm 0.9 Ag 0.1 Mn 2 O 5 ) of perovskite-type and mullite crystal phases were synthesized for the catalytic oxidation of CO and C 3 H 8 . The Sm 0.9 Ag 0.1 Mn 2 O 5 composition showed the highest catalytic activity among the series of solids, especially for the CO oxidation to CO 2 with T 50 and T 90 values of 60 and 95 °C, respectively. The catalysts were characterized by powder XRD, Raman, BET, XPS, and H 2 -TPR. It was found that the catalytic performance of the solids was correlated well with their redox properties. Synergetic effects between Ag-related species and the mullite phase resulted in more active surface oxygen species and remarkably lowered the reduction temperature of the Sm 0.9 Ag 0.1 Mn 2 O 5 solid.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMIE INGENIEUR TECHNIK
·
2021
·
IF 1.672
Luxi Lyu,Houxiao Wu,Libo Li,Yanying Wei,Haihui Wang
Metal-organic frameworks (MOFs) show great potential for adsorption separation. However, MOFs' flexibility may influence their adsorption behaviors. Here, for the first time we prepare ZIF-8 powder dominated with stiffened ZIF-8_Cm phase under an external E-field. By comparison, we find that the flexibility of ZIF-8 has little influence in equilibrium-based separation behavior for C 3 H 6 /C 3 H 8 . However, the stiffened ZIF-8 formed in E-field presents an obviously decreased diffusion rate for C 3 H 8 , whose C 3 H 6 /C 3 H 8 kinetic-based separation factor is around 2.5 times higher than that of the traditional ZIF-8 powder.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Ping Yang,Xiuhong Meng,Penghu Guo,Rujin Zhou,Youhua Zhang,Shui Cao,Dan Zhang,Hongbing Ji,Linhai Duan
Two critical characteristics for gas adsorption and separation are the porosity and open metal sites of adsorbents. The Cu–BTC (BTC = benzene–1,3,5–tricarboxylate) structure was tailored using a template synthesis technique to increase the separation performance for C 3 H 6 /C 3 H 8 mixtures. The three hierarchical porous frameworks, Cu x O y @HP–Cu–BTC, synthesized using a cationic surfactant (cetyltrimethylammonium bromide (CTAB)), a neutral organic amine (N,N–dimethyltetradecylamine (N,N)), and an anionic surfactant (sodium dodecylbenzene sulfonate (SDBS)) as the template, Cu x O y @HP–Cu–BTC(SDBS) exhibited the best performance, with a C 3 H 6 adsorption capacity of 6.679 mmol g −1 , which was significantly greater than that of C 3 H 8 (5.721 mmol g −1 ). Cu x O y @HP–Cu–BTC(SDBS) has an ideal ultra–microporous structure that encloses C 3 H 6 molecules precisely while rejecting slightly bigger C 3 H 8 molecules, and C 3 H 6 interacts strongly with unsaturated metal sites through particular π–Cu bonds. According to the ideal adsorbed solution theory (IAST), the adsorption selectivity of C 3 H 6 /C 3 H 8 was 63.322, which is more than that of the reference adsorbent Cu–BTC. Additionally, the breakthrough studies shown that Cu x O y @HP–Cu–BTC(SDBS) has a good dynamic performance for the effective separation of the C 3 H 6 /C 3 H 8 mixture.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Ruijie Zhu,Leilei Kang,Lin Li,Xiaoli Pan,Hua Wang,Yang Su,Guangyi Li,Hongkui Cheng,Rengui Li,Xiao Yan Liu,Aiqin Wang
Catalytic oxidation is a commonly employed technology in the industry for removing volatile organic compounds (VOCs) due to its exceptional efficiency under mild operating conditions. Although supported Pt-based nano-catalysts are recognized widely as one of the most promising and extensively used industrial catalysts for VOC abatement, their practical application, and development are restricted by their exorbitant cost. Single-atom catalyst (SAC) with maximized metal utilization and exclusive electronic character has been explored extensively in various catalytic reactions. However, Pt SAC is usually deemed to be inactive in hydrocarbon oxidation reactions in thermal catalysis, compared with its nanoparticle counterpart. Here, we demonstrate that the WO 3 -TiO 2 supported Pt SAC (Pt 1 /WO 3 -TiO 2 ) exhibits much higher activities than the corresponding nanoparticle catalyst (Pt NP /WO 3 -TiO 2 ) in photo-thermo catalytic oxidation of C 3 H 8 and C 3 H 6 , which represent different kinds of typical VOCs. A key finding is that the activities of Pt 1 /WO 3 -TiO 2 and Pt NP /WO 3 -TiO 2 can be accelerated in photo-thermo catalytic C 3 H 8 oxidation by overcoming oxygen poisoning. Upon the light irradiation, the apparent active energy ( E a ) of the Pt 1 /WO 3 -TiO 2 and Pt NP /WO 3 -TiO 2 decline from 116 to 60 kJ·mol −1 and from 103 to 30 kJ·mol −1 , respectively, substantiating their effectiveness in photo-thermo catalysis. Notably, a substantially higher reaction rate of 3792 μmol∙g Pt −1 ∙s −1 on the Pt 1 /WO 3 -TiO 2 is achieved, which should be a benchmark for C 3 H 8 oxidation. More intriguingly, photo-thermo catalytic C 3 H 6 oxidation on the Pt NP /WO 3 -TiO 2 is prohibited due to the strong adsorption-induced C 3 H 6 poisoning on the Pt nanoparticles, for which the E a of the Pt NP /WO 3 -TiO 2 catalyst for C 3 H 6 oxidation is maintained at approximately 55 kJ·mol −1 , regardless of the light irradiation. In comparison, the C 3 H 6 poisoning on the Pt 1 /WO 3 -TiO 2 can be mitigated by light illumination, where the E a of the Pt 1 /WO 3 -TiO 2 catalyst for C 3 H 6 oxidation dramatically reduced from 49 to 16 kJ·mol −1 , signifying that the high energy barrier of C 3 H 6 oxidation can be mediated by the light. Profiting from the apt affinity between C 3 H 6 and Pt single atoms, the photogenerated electrons accumulated on the Pt single atoms produce repulsive force towards the electron-rich C 3 H 6 molecules, which is conducive to the C 3 H 6 desorption from the Pt 1 /WO 3 -TiO 2 . Therefore, the Pt 1 /WO 3 -TiO 2 exhibits enhanced activity in photo-thermo catalytic C 3 H 6 oxidation. This study exemplifies that the advantages of SAC are not only saving the consumption of precious metals but also discovering new catalytic reactions on the account of the specific electronic characteristic. Download: Download high-res image (85KB) Download: Download full-size image
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Yumeng Xu,Rongzhou Chen,Hailian Tang,Lu Yan,Fei Huang,Ming Tian,Kaibao Wu,Yanliang Zhou,Jian Lin,Ying Zheng,Xiaodong Wang
Promoting the thermal stability of supported noble metal catalysts under harsh conditions remains challenging for the modern chemistry industry. Herein, Fe-substituted hexaaluminate supported Pt catalysts (Pt/BaFeAl11O19) were synthesized and treated with high temperature at 800 °C under different atmospheres. The Pt particles showed severe sintering under an oxidative atmosphere but high stability under reductive conditions. Interestingly, Pt/BaFeAl11O19 pre-reduced at high temperature possessed improved anti-sintering ablility during oxidative annealing. The characterization results demonstrate that oxygen vacancies were facilely formed under an H2 atmosphere to favor the formation of coating layers on Pt nanoparticles. This structure helps retain oxygen vacancies during subsequent oxidative calcination, contributing to promoted stability. The high thermal stability of Pt particles coupled with the easy generation of Fe2+ sites in Pt/BaFeAl11O19 resulted in excellent catalytic performance for CO and C3H8 oxidation after cycling hydrothermal aging at 800 °C.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Jingxian Hua,Chang Li,Hongxu Tao,Lei Wang,Eryue Song,Haiqian Lian,Chongqing Wang,Jinlong Jiang,Yichang Pan,Weihong Xing
Polymer coating post-treatment strategy of the zeolitic imidazolate framework (ZIF) membranes offers a versatile and feasible opportunity to restrict the intrinsic flexibility of ZIF framework and improve their gas separation performance. Herein, two different coating methods (Vacuum-assisted drip coating (VADC) and Static drip coating (SDC)) are utilized to prepare PDMS/ZIF-8 composite membranes based on ZIF-8 membranes with different compactness (high, medium and low-quality membrane) for investigating the effect of the contact area between PDMS layer and ZIF-8 membrane on C 3 H 6 /C 3 H 8 separation performance of PDMS/ZIF-8 composite membranes. The results reveal that the increase of the contact between PDMS layer and ZIF-8 membrane can enhance the contact confinement effect on the flexibility of ZIF-8 framework, resulting in a higher improvement of the separation performance for C 3 H 6 /C 3 H 8 of PDMS/ZIF-8 composite membranes with pressure. The prepared composite membrane based on VADC method showed a significant improvement in C 3 H 6 /C 3 H 8 separation factor (77–102) with slight increase in C 3 H 6 permeance (about 10%) at feed pressure of 7 bar. Moreover, this facile vacuum-assisted drip strategy attenuated the impact of the quality of ZIF-8 membranes on fabrication reproducibility of the composite membranes, which can withstand high pressure. Therefore, this work advances ZIF-8 membrane moving forward to industrial C 3 H 6 /C 3 H 8 separation.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Peng Hu,Jun Han,Jie Zhou,Hao Wang,Chao Xiong,Hao Liu,Xiantai Zhou,Yongqing Wang,Hongbing Ji
Efficient separation of propylene/propane (C 3 H 6 /C 3 H 8 ) is an imperative and extremely challenging process in the petrochemical industry due to their similar physicochemical characters. Known tactics mainly concentrate on unilateral thermodynamic or kinetic driven. Here, we report the efficient separation of C 3 H 6 /C 3 H 8 through cooperative equilibrium-kinetic synergetic effect in a nodes-engineered Zr-MOF scaffold (1to). The grafted -CF 3 motif with different isomers and resultant aperture chemistry awards 1to a late-model paradigm for efficient separation of C 3 H 6 /C 3 H 8 . Detailly, confined -CF 3 group having the role of H-bonding acceptor can result in improved adsorption enthalpy ( Q st ) of 38.1 kJ mol −1 , ideal adsorbed solution theory (IAST) selectivity of 80 and experimental selectivity of 25, respectively, indicating a marked thermodynamic driven for trapping C 3 H 6 . Besides, the contracted cross-sectional size and eligible pore shape of 1to could be judiciously adjusted through rationally engineering the pore microenvironment, yielding a topmost simulated diffusion selectivity of 408, which was 40.8 times higher than that of the pristine 1 example (10), effectively enabling the swift diffusion behavior of C 3 H 6 . Modeling simulations and breakthrough experiments confirmed the excellent C 3 H 6 /C 3 H 8 separation performance of 1to. This work successfully developed a novel nodes-engineered strategy for C 3 H 6 capture through equilibrium-kinetic synergetic effect, anticipating to set a new benchmark for gas separation and affording constructive guidance for tailoring delicate aperture chemistry.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Wei Chen,Juan Zheng,Yarong Fang,Yutao Wang,Jinpeng Hu,Yuhua Zhu,Xiaoxiao Zhu,Weihao Li,Qian Zhang,Chuanqi Pan,Baojian Zhang,Xiaofeng Qiu,Sibo Wang,Shuang Cui,Jinlong Wang,Jinsong Wu,Zhu Luo,Yanbing Guo
Typically, SO2 unavoidably deactivates catalysts in most heterogeneous catalytic oxidations. However, for Pt-based catalysts, SO2 exhibits an extraordinary boosting effect in propane catalytic oxidation, but the promotive mechanism remains contentious. In this study, an in situ-formed tactful (Pt–S–O)-Ti structure was concluded to be a key factor for Pt/TiO2 catalysts with a substantial SO2 tolerance ability. The experiments and theoretical calculations confirm that the high degree of hybridization and orbital coupling between Pt 5d and S 3p orbitals enable more charge transfer from Pt to S species, thus forming the (Pt–S–O)-Ti structure with the oxygen atom dissociated from the chemisorbed O2 adsorbed on oxygen vacancies. The active oxygen atom in the (Pt–S–O)-Ti active structure is a robust site for C3H8 adsorption, leading to a better C3H8 combustion performance. This work can provide insights into the rational design of chemical bonds for high SO2 tolerance catalysts, thereby improving economic and environmental benefits.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Jinshi Dong,Ting Li,Shengtong Li,Panpan Chang,Qianqian Jin,Jiaqiang Yang,Zhuangzhuang Lai
CO and C3H8, as typical inorganic and organic gaseous pollutants, respectively, require distinct oxidation catalysts for efficient conversion due to their unique properties. In this work, Pt catalysts with different crystal phases of TiO2 (anatase and rutile) as supports were fabricated and investigated for CO oxidation and C3H8 combustion. The surface nature of TiO2 dramatically affects the local environment and electronic properties of supported Pt. Pt-TiO2(R) exhibited superior activity for CO oxidation, whereas Pt-TiO2(A) showed higher reactivity for C3H8 total oxidation. It is concluded that Pt-TiO2(R) contains more oxygen vacancies at the interfacial Pt perimeter sites than Pt-TiO2(A) after reduction pretreatments, which facilitates CO oxidation through the Mars–van Krevelen (MvK) mechanism. The electron-deficient Pt in Pt-TiO2(A) promotes the adsorption and activation of C3H8, and the amount of charge transfer between Pt and adsorbate intermediates during C3H8 oxidation determines the preference of C-C cleavage or dehydrogenation. Lower charge transfer in Pt-TiO2(A) makes C–C cleavage more efficient and contributes to the total oxidation of C3H8. This work emphasizes the importance of engineering material’s local environment and electronic structure to design high-performance oxidation catalysts.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Changhai Fan,Zhengwang Xia,Haiqian Lian,Luogang Wu,Eryue Song,Jingxian Hua,Li Shen,Rujing Hou,Yichang Pan,Weihong Xing
The ZIF-8 membrane has emerged as a promising candidate for C 3 H 6 /C 3 H 8 separation. However, the feasibility of ZIF-8 membranes for applications has rarely been investigated with gas provided directly by the industry sector. Herein, the C 3 H 6 /C 3 H 8 mixture collected from the backend of the Hydrogen Peroxide to Propylene Oxide (HPPO) process was applied as feed gas to examine the separation performance of tubular ZIF-8 membranes. The membranes exhibited excellent separation performance and long-term stability under 9 bar and 50 °C. Noticeably, upon scaling up to a membrane area of 452.16 cm 2 by connecting six three-channel modules in series (multi-step membrane), its separation performance satisfied the C 3 H 6 circulation requirements during the HPPO process (purity ≥97.5 % and recovery rate ≥85 %). Furthermore, a simulation of membrane operation under industrial working conditions (22 bar and 56.3 °C) was performed. By fixing the separation factor at 15, a minimum membrane area of 800 m 2 met the requirements at the cost of membrane permeance with 120 GPU. The corresponding economic calculation indicated a maximum of 91.8 % annual capital cost saving compared with the distillation process, paving the way for the practical application of membranes.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale Research Letters
·
2020
·Vol. 15
·期 1
·1-15
·
IF 3.578
Fan Li,Sun Qi,Zheng Wei,Tang Qinyuan,Zhang Ting,Tian Mengkui
The rutile Sn x Ti 1− x O 2 ( x = 0, 0.33, 0.5, 0.67, 1) solid solution was synthesized by a one-step hydrothermal method, in which tetrabutyl titanate and Tin (IV) chloride pentahydrate were used as raw materials. A series of Ru/Sn x Ti 1− x O 2 were then prepared by the impregnation process in RuCl 3 to investigate the performance and stability of CO and C 3 H 8 oxidation. These catalysts were characterized through XRD, N 2 adsorption-desorption, FT-IR, TEM, XPS, H 2 -TPR, and O 2 -TPD techniques. The effect of Sn/Ti molar ratio and hydrothermal condition on the low-temperature catalytic oxidized performance and stability of Ru/Sn x Ti 1− x O 2 were investigated. The results indicated that Ru/Sn 0.67 Ti 0.33 O 2 catalyst showed an excellent activity and stability at low temperatures. The CO conversion reached 50% at 180 °C and 90% at 240 °C. Besides, the C 3 H 8 conversion reached 50% at 320 °C, the complete conversion of C 3 H 8 realized at 500 °C, and no deactivation occurs after 12 h of catalytic reaction. The excellent low-temperature activity and stability of the Ru/Sn 0.67 Ti 0.33 O 2 were attributed to the following factors. Firstly, XRD results showed that Sn 4+ was successfully introduced into the lattice of TiO 2 to replace Ti 4+ forming a homogeneous solid solution (containing –Sn 4+ –O–Ti 4+ – species), which was consistent with TEM and N 2 adsorption-desorption results. The introduction of Sn could suppress the growth of anatase crystal and promote the formation of rutile phase, and this phase transition was helpful to improve the low-temperature activity of the catalysts. Secondly, TEM images showed that ultrafine Ru nanoparticles (~ 5 nm) were dispersed on Sn 0.67 Ti 0.33 O 2 support, suggesting that the formation of Sn x Ti 1− x O 2 solid solution was beneficial to the dispersion of Ru particles.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
·
2015
·Vol. 38
·期 2
·291-296
·
IF 2.442
Chen Zhou,Yexin Zhang,Lingjun Hu,Hongfeng Yin,Wei Guo Wang
Mn-doped La 0.8 Sr 0.2 CoO 3 perovskite oxides (La 0.8 Sr 0.2 Co 1– x Mn x O 3 ; x = 0, 0.1, 0.3, 0.5) were synthesized by a modified sol-gel method. The phase-pure oxides were obtained. CoO and carbonates were formed on the surface of La 0.8 Sr 0.2 CoO 3 . With increasing doping content, these impurities were reduced while the stability of the perovskite structure was improved. The valence state of B-site ions and the amount of absorbed oxygen were influenced by Mn doping. The catalytic activity of the perovskite catalysts was investigated for CO oxidation and simultaneous removal of CO, C 3 H 8 , and NO. For CO and NO removal, La 0.8 Sr 0.2 Co 0.9 Mn 0.1 O 3 exhibited the best performance. For C 3 H 8 removal, the reactivity was promoted linearly with the doping content. The structure-activity relationship is also discussed.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）