Nanoscale
·
2024
·
IF 5.8
Heyun Lin,Wenzhe Zhang,Huachen Shen,Hailing Yu,Yunlei An,Tiejun Lin,Liangshu Zhong
The catalytic behavior of CO hydrogenation can be modulated by metal–support interactions, while the role of the support remains elusive. Herein, we demonstrate that the presence of strong metal–support interactions (SMSI) depends strongly on the crystal phase of TiO2 (rutile or anatase) and the treatment conditions for the TiO2 support, which could critically control the activity and selectivity of Ru-based nanocatalysts for CO hydrogenation. High CO conversion and olefin selectivity were observed for Ru/rutile-TiO2 (Ru/r-TiO2), while catalysts supported by anatase (a-TiO2) showed almost no activity. Characterization confirmed that the SMSI effect could be neglected for Ru/r-TiO2, while it is dominant on Ru/a-TiO2 after reduction at 300 °C, resulting in the coverage of Ru nanoparticles by TiOx overlayers. Such SMSI could be suppressed by H2 treatment of the a-TiO2 support and the catalytic activity of the as-obtained Ru/a-TiO2(H2) can be greatly elevated from almost inactive to >50% CO conversion with >60% olefin selectivity. Further results indicated that the surface reducibility of the TiO2 support determines the SMSI state and catalytic performance of Ru/TiO2 in the CO hydrogenation reaction. This work offers an effective strategy to design efficient catalysts for the FTO reaction by regulating the crystal phase of the support.
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2022
·Vol. 12
·期 5
·480
·
IF 4.501
Xiuyu Sun,Zhenwei Wang,Wei Yan,Chuangan Zhou
The application potential of Pt/Ti4O7has been reported, but the lack of research on the relationship between Pt loading, MSI, and catalytic activity hinders further development. Micron-sized Ti4O7powders synthesized by a thermal reduction method under an H2atmosphere were used as a support material for Pt-based catalysts. Using a modified polyol method, Pt/Ti4O7-5, Pt/Ti4O7-10, and Pt/Ti4O7-20 with different mass ratios (Pt to Pt/Ti4O7is 0.05, 0.1, 0.2) were successfully synthesized. Uniformly dispersed platinum nanoparticles exhibit disparate morphologies, rod-like for Pt/Ti4O7-5 and approximately spherical for Pt/Ti4O7-10 and Pt/Ti4O7-20. Small-angle deflections and lattice reconstruction induced by strong metal–support interactions were observed in Pt/Ti4O7-5, which indicated the formation of a new phase at the interface. However, lattice distortions and dislocations for higher loading samples imply the existence of weak metal–support interactions. A possible mechanism is proposed to explain the different morphologies and varying metal–support interactions (MSI). With X-ray photoelectron spectroscopy, spectrums of Pt and Ti display apparent shifts in binding energy compared with commercial Pt-C and non-platinized Ti4O7, which can properly explain the changes in absorption ability and oxygen reduction reaction activity, as described in the electrochemical results. The synthetic method, Pt loading, and surface coverage of the support play an important role in the adjustment of MSI, which gives significant guidance for better utilizing MSI to prepare the target catalyst.Keywords:platinum;titanium suboxide;electrocatalyst;SMSI
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 19
·6879
·
IF 4.6
Tiantian Zhang,Jiacheng Xu,Yan Sun,Shiyu Fang,Zuliang Wu,Erhao Gao,Jiali Zhu,Wei Wang,Shuiliang Yao,Jing Li
Pt-based catalysts exhibit unique catalytic properties in many chemical reactions. In particular, metal–support interactions (MSI) greatly improve catalytic activity. However, the current MSI mechanism between platinum (Pt) and the support is not clear enough. In this paper, the interaction of 1 wt% Pt nanoparticles (NPs) onβ-MnO2in carbon monoxide (CO) oxidation was studied. The Pt onβ-MnO2inhibited CO oxidation below 210 °C but promoted it above 210 °C. A Pt/β-MnO2catalyst contains more Pt4+and less Pt2+. The results of operando DRIFTS-MS show that surface-terminal-type oxygen (M=O) plays an important role in CO oxidation. When the temperature was below 210 °C, Mn=O consumption on Pt/β-MnO2was less thanβ-MnO2due to Pt4+inhibition on CO oxidation. When the temperature was above 210 °C, Pt4+was reduced to Pt2+, and Mn=O consumption due to CO oxidation was greater thanβ-MnO2. The interaction of Pt andβ-MnO2is proposed.Keywords:metal–support interaction;CO oxidation;terminal-type oxygen;bridge-type oxygen;Pt;MnO2
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
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2022
·Vol. 12
·期 9
·955
·
IF 4.501
Beilei Cui,Hua Wang,Qingfeng Ge,Xinli Zhu
A series of rutile TiO2-supported Ni catalysts with varying Ni sizes were prepared and reduced at 650 °C to explore the effect of Ni size on the strong metal–support interactions (SMSI) and its consequences on the hydrodeoxygenation (HDO) of m-cresol at 350 °C and atmospheric pressure. When the Ni size increases from 4 to 29.1 nm, the SMSI becomes stronger, e.g., the thickness of the TiOxoverlayer and the coverage extent of TiOxon the Ni particle surface increase. Direct deoxygenation to toluene is the dominant pathway on Ni/TiO2catalysts with varying Ni loadings, with almost no CH4being formed. These results indicate that the TiOxoverlayer significantly alters the property of Ni. That is, the C-C hydrogenolysis activity on bare Ni is completely inhibited due to SMSI, while the deoxygenation activity is improved at the Ni-TiOxinterfacial perimeter sites. Meanwhile, the turnover frequency of HDO on small Ni particles of 4 nm is > 2 times higher than that on large Ni particles of 29.1 nm, indicating that the small Ni particle with moderate SMSI appears to be optimal for the direct deoxygenation of m-cresol to toluene. The results suggest HDO activity may be enhanced by tuning the metal particle size and SMSI degree.Keywords:Ni/TiO2;rutile;strong metal-support interactions;m-cresol;hydrodeoxygenation
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Kang Li,Chunlei Pei,Xinyu Li,Sai Chen,Xianhua Zhang,Rui Liu,Jinlong Gong
The modulation of the interaction between the active metal and the underlying support material plays a key role and remains a challenge in many important catalytic reactions. This paper describes a new method for the modification of Ni/Al 2 O 3 by La 2 O 2 CO 3 , which is responsible for modulating the interaction between Ni and the Al 2 O 3 support. When La 2 O 2 CO 3 is loaded on the Al 2 O 3 support as a La 2 O 3 precursor, combined with XRD, H 2 -TPR, H 2 -pluse chemisorption, Raman spectroscopy and TEM characterization, it is found that La 2 O 2 CO 3 can prevent Ni from entering the alumina support and forming NiAl 2 O 4 . This strategy allows more Ni to be reduced and exposed as active sites. Consequently, the La 2 O 2 CO 3 modified Ni/Al 2 O 3 exhibited superior activity with respect to the reference La 2 O 3 modified Ni/Al 2 O 3 and original Ni/Al 2 O 3 in dry reforming of methane (DRM). At the same time, La can cover the acidic sites of alumina and increase the alkalinity of the catalyst, thereby promoting carbon dioxide adsorption and activation, and inhibiting carbon deposition. In addition, the introduction of La also inhibits the sintering of Ni under harsh reaction conditions by enhancing the interaction between Ni metal and the support. This modification method can simultaneously improve the reactivity and stability of the catalyst by altering the interaction between the metal and the support.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
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2019
·
IF 2.846
Wenfeng Han,Zhi Li,Huazhang Liu
La 2 Ce 2 O 7 nanoparticles were prepared by citric acid complexation method followed by calcination at varied temperatures. Then, supported with 4 wt% Ru, they were evaluated as the catalysts for ammonia synthesis under conditions similar with industry. With La 2 Ce 2 O 7 being calcinated at 700 or 800 °C, the experimental results indicate that the Ru/La 2 Ce 2 O 7 catalyst exhibits much higher ammonia concentration or ammonia synthesis rate than that of Ru/CeO 2 and Ru/La 2 O 3 . In addition, Ru/La 2 Ce 2 O 7 possesses high stability under over-heating test. In the absence of any promotor, ammonia concentration of Ru/La 2 Ce 2 O 7 catalyst approaches 14% at 450 °C, GHSV of 10000 h −1 and pressure of 10 MPa. The rate-determining step of ammonia synthesis, dissociation of N 2 is significantly facilitated by the strong metal–support interaction (SMSI) between Ru and La 2 Ce 2 O 7 . Due to the interaction, La 2 Ce 2 O 7 tends to donate electrons to Ru, resulting in the high electron density over the surface of Ru active sites which is favorable for the dissociation of N 2 . Consequently, high activity is achieved.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2021
·Vol. 8
·期 22
·2102207
·
IF 16.806
Sin-Yi Pang,Weng-Fu Io,Jianhua Hao
Supported metallic nanoparticles render highly tunable physical and chemical properties to mixed-dimensionality materials in electrocatalysts. However, some supports are susceptible to being dissolved in acidic solution or are unstable in ambient air. The development of high-performance catalysts has been facing the major hurdles of the sluggish activity in alkaline solution and requesting high energy to stabilize the nanoparticles on their supports, challenging the pH-universality and the applicability of the supported metallic nanoparticles. Here, a one-step strategy is proposed to modulate the growth of Pt quantum dots (QDs) on HF-free MXene under atomic-level by a low-temperature metal–support interaction reaction. By controllable tailoring in the morphology and strain induced by terminations, Pt (111) QDs with a sub-nanoscale size of 1.15 nm are grown as 0D/1D heterostructure to overcome the restrictions of employing reduction gas and high annealing temperature. The catalyst exhibits a low overpotential of 33.3 mV for acidic solution, while 65.1 mV for alkaline solution at a specific current density of 10 mA cm −2 . This study not only paves a scalable pathway to developing cost-efficient catalysts in moderate conditions, but also demonstrates an effective surface modulation strategy for 0D/1D heterostructures.
研究领域:
材料科学
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电催化
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Li Ruili,Liu Lin,Ju Xiaohua,Feng Ji,Wang Jiemin,Guo Jiangping,He Teng,Chen Ping
The essential role of metal–support interaction in ammonia synthesis was investigated by using a Pr 6 O 11 supported Ru nanoparticles (NPs) catalyst system. Loading of Ru NPs onto the Pr 6 O 11 support with relatively low surface area yields similar metal dispersion with respect to conventional SiO 2 support. The Ru NPs on the Pr 6 O 11 was found to exhibit excellent catalytic performance in ammonia synthesis, superior to free-standing Ru NPs and Ru NPs on conventional SiO 2 support. Detailed structure analysis results reveal that the superior activity of Ru/Pr 6 O 11 can be attributed to the enhanced interaction between the Ru NPs and Pr 6 O 11 , which can modulate the electronic structure of Ru NPs and trigger catalytic ammonia synthesis over Ru NPs on Pr 6 O 11 . Furthermore, nitrogen isotope exchange experiment reveals that superior nitrogen dissociation ability is essential for the excellent activity and intrinsic activity of Ru/Pr 6 O 11 in ammonia synthesis. These findings demonstrate that Pr 6 O 11 can be used as a new kind of support for preparation of efficient Ru-based catalysts for ammonia synthesis, and also open up opportunities for design of Pr 6 O 11 supported metal catalysts for other catalytic reactions. Graphitical Abstract Interaction between the Ru NPs and Pr 6 O 11 can modulate the electronic structure of Ru NPs and trigger catalytic ammonia synthesis over Ru NPs on Pr 6 O 11 .
研究领域:
催化化学
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材料科学
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物理化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
·
IF 3.764
Min Zhao,Ziang Zhao,Yuan Lyu,Wei Lu,Ming Jin,Tao Liu,Hejun Zhu,Yunjie Ding
Suitable metal–support interaction is of great significance for the supported Fischer–Tropsch catalyst. Herein, we synthesized a series of porous spinel MAl2O4 (M = Co, Mg, Zn) together with Al2O3, via a sol–gel method and used them as supports for the Co-based Fischer–Tropsch synthesis (FTS) catalyst to investigate the influence of metal–support interaction on Co dispersity, reducibility, and catalytic performance. The catalytic performance showed that 15Co/CoAl2O4 had the highest activity and C5+ selectivity, as well as favorable stability during 1000 h lifetime testing. The catalysts were characterized by physisorption, chemisorption, HRTEM, XPS, and TPSR. The results indicated that 15Co/CoAl2O4 showed weaker metal–support interaction than 15Co/MgAl2O4 and 15Co/Al2O3, which was considered as the key factor for its higher reducibility and CO dissociation ability, contributing to the higher CO conversion. The higher Co dispersity on CoAl2O4 resulted from the smaller particle size of Co species on CoAl2O4, contributing to the higher activity of 15Co/CoAl2O4 than that of 15Co/ZnAl2O4. The higher C5+ selectivity on 15Co/CoAl2O4 and 15Co/ZnAl2O4 than that on 15Co/MgAl2O4 and 15Co/Al2O3 was verified to benefit from the appropriate H2/CO adsorption ability, which was significantly affected by metal–support interaction.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Qiufeng Liu,Kaihang Sun,Kun Lu,Xingwei Xie,Longzhou Zhang,Young Dok Kim,Zhongyi Liu,Zhikun Peng
Metal-support interaction (MSI) is an efficient strategy to modulate the distribution of active metal with different electronic states over the oxide-supported metal catalysts. However, the intrinsic correlation between the intensity of MSI and the electronic structure of supported metals remains inadequate. In this work, the intensity of MSI over the Cu/Y 2 O 3 catalyst was tuned by the calcination temperature, which regulated the distribution of Cu 0 , Cu + and Cu 2+ species. The Cu/Y 2 O 3 catalyst with the highest amount of Cu + exhibits the superior performance of reverse water–gas shift reaction. Due to the enhanced H 2 activation and promoted charge transfer at the interfacial Cu + /Y 2 O 3 site based on the experimental characterizations, the CO formation rate reached 220 mmol CO g cat −1 h −1 at 500 °C. The present work provides an efficient way to regulate the supported metal species with the specific electronic state.
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qiang Fu,Lei Lin,Tao Wu,Qinghua Zhang,Xianjie Wang,Lingling Xu,Jun Zhong,Lin Gu,Zhihua Zhang,Ping Xu,Bo Song
Precious metals (Pt, Ir, Ru, and so on) and related compounds usually demonstrate superb catalytic activity for electrochemical hydrogen production. However, scarcity and stability are still challenges for hydrogen evolution reaction, even for single-atomic-site electrocatalysts. Herein, a fluorine (F) doping strategy is proposed to enhance the strong metal–support interaction between the F-doped Ni3N support and the loaded ruthenium (Ru) species. Via synergistically modulating both the Ru loading amount and F doping concentration, outstanding HER activity was achieved in Ru@F–Ni3N with an overpotential (η) of 115 mV at 100 mA cm–2, superior to the benchmark Pt/C (η = 201 mV). Density functional theory simulation in combination with X-ray photoelectron spectra and X-ray absorption spectroscopy characterizations convincingly demonstrate that, with the strongest electronegativity, F doping could effectively stabilize Ru atoms doped in the F–Ni3N substrate and simultaneously reduce the H bonding strength, which accelerated the desorption of H2. These findings provide a facile strategy to modulate both catalytic activities and stabilities of heteroatom-loaded catalytic materials.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yarong Bai,Houlin Wang,Chao Jin,Chuan Gao,Shangchao Xiong,Zhengjun Gong,Yue Peng,Junhua Li
Precision modulation of metal-support interactions is essential for optimizing catalytic activity and selectivity in automotive exhaust treatment. In this study, we systematically regulate the strength of Pt-CeO 2 interaction by altering Pt anchoring strategies on Al 2 O 3 , thereby achieving a controlled balance between NO x reduction efficiency and by-product formation. Comprehensive structural and spectroscopic analyses reveal that increasing the interaction strength (PtCeAl-mix
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
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）