ACS Catalysis
·
2021
·
IF 13.084
Shaofeng Liu,Haifeng Qi,Junhui Zhou,Wei Xu,Yiming Niu,Bingsen Zhang,Yang Zhao,Wei Liu,Zhimin Ao,Zhichong Kuang,Lin Li,Meng Wang,Junhu Wang
Classical strong metal–support interaction (SMSI) has attracted intensive attention in the heterogeneous catalysis field; however, its crystalline TiOx overlayer and reversible feature often curtail the effect of classical SMSI on enhancing the catalytic performance of supported metal catalysts in oxidation reactions, especially at elevated temperatures. Here, we report the evidence that Pt nanoparticles can be encapsulated by an amorphous and permeable TiOx cover layer in Pt/TiO2 catalysts under an oxidative atmosphere, where the keys are the utilization of melamine, followed by annealing in nitrogen flow and further calcination at 800 °C in air. More importantly, the formed overlayer is stabilized against re-oxidation at 400–600 °C in air, in sharp contrast to the retreat of the TiOx overlayer by subsequent oxidation treatment in classical SMSI. Such an extraordinary strategy is further demonstrated on titania-supported Pd and Rh nanoparticles, paving a promising way for designing supported platinum group metal-based catalysts with high activity and stability.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Science Advances
·
2017
·Vol. 3
·期 10
·
IF 0
Hailian Tang,Yang Su,Bingsen Zhang,Adam F. Lee,Mark A. Isaacs,Karen Wilson,Lin Li,Yuegong Ren,Jiahui Huang,Masatake Haruta,Botao Qiao,Xin Liu,Changzi Jin,Dangsheng Su,Junhu Wang,Tao Zhang
Supported metal catalysts play a central role in the modern chemical industry but often exhibit poor on-stream stability. The strong metal–support interaction (SMSI) offers a route to control the structural properties of supported metals and, hence, their reactivity and stability. Conventional wisdom holds that supported Au cannot manifest a classical SMSI, which is characterized by reversible metal encapsulation by the support upon high-temperature redox treatments. We demonstrate a classical SMSI for Au/TiO2, evidenced by suppression of CO adsorption, electron transfer from TiO2 to Au nanoparticles, and gold encapsulation by a TiOx overlayer following high-temperature reduction (reversed by subsequent oxidation), akin to that observed for titania-supported platinum group metals. In the SMSI state, Au/TiO2 exhibits markedly improved stability toward CO oxidation. The SMSI extends to Au supported over other reducible oxides (Fe3O4 and CeO2) and other group IB metals (Cu and Ag) over titania. This discovery highlights the general nature of the classical SMSI and unlocks the development of thermochemically stable IB metal catalysts.
研究领域:
催化化学
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材料科学
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DOI
PubMed
Journal of Energy Chemistry
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2021
·
IF 9.676
Yaoxin Wang,Jiandian Wang,Ping Zheng,Changyong Sun,Junyin Luo,Xiaowei Xie
Propane dehydrogenation (PDH) provides an alternative route for producing propylene. Herein, we demonstrates that h-BN is a promising support of Pt-based catalysts for PDH. The Pt catalysts supported on h-BN were prepared by an impregnation method using Pt(NH 3 ) 4 (NO 3 ) 2 as metal precursors. It has been found that the Pt/BN catalyst undergoing calcination and reduction is highly stable in both PDH reaction and coke-burning regeneration, together with low coke deposition and outstanding propylene selectivity (99%). Detailed characterizations reveal that the high coke resistance and high propylene selectivity of the Pt/BN catalyst are derived not only from the absence of acidity on BN support, but also from the calcination-induced and reduction-adjusted strong metal-support interaction (SMSI) between Pt and BN, which causes the partial encapsulation of Pt particles by BO x overlayers. The BO x overlayers can block the low-coordinated Pt sites and constrain Pt particles into smaller ensembles, suppressing side reactions such as cracking and deep dehydrogenation. Moreover, the BO x overlayers can effectively inhibit Pt sintering by the spatial isolation of Pt during periodic reaction-regeneration cycles. In this work, the catalyst support for PDH is expanded to nonoxide BN, and the understanding of SMSI between Pt and BN will provide rational design strategy for BN-based catalysts.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 9
·3579-3588
·
IF 8.307
Jianjun Zhou,Tian Wang,Cheng Cheng,Fan Pan,Yunqing Zhu,Hongrui Ma,Junfeng Niu
Electrocatalytic oxidation is regarded as an effective technique for decomposing refractory organic compounds like perfluorooctanoic acid (PFOA). However, achieving highly efficient and long-life electrodes is still a great challenge. Herein, Ti/RuO2–IrO2@Pt anodes consisting of Pt4+ and Pt0 species were fabricated by combining modified microemulsion technology with a calcination process, in which Pt nanoparticles were highly dispersed and encapsulated in Ru–Ir composite oxides to form a strong metal–support interaction (SMSI) structure. The as-constructed SMSI layer on the Ti/RuO2–IrO2@Pt anode resulted in the improvement of the charge transfer capability and also increased the degradation (99.30%) and mineralization (91.32%) of PFOA during the electrochemical oxidation process. Notably, the service lifetime of Ti/RuO2–IrO2@Pt anodes was remarkably improved from 24 to 42.3 h compared to commercial Ti/RuO2–IrO2 anodes. Moreover, the possible degradation mechanism of PFOA was also speculated through the detection of short-chain perfluorocarboxylic acids and reactive radicals. These results not only revealed that the concept and methodology of SMSI could be an effective way for constructing highly efficient and stable electrocatalysts but also greatly advanced fundamental understanding.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Mingjie Huang,Sisi Peng,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Tao Zhou
This study has revealed how the strong metal-support interaction (SMSI) between carbon nanotubes (CNTs) and Mn 0.65 Fe 2.35 O 4 (MnFeO) in boosting peroxymonosulfate (PMS) activation for rapid sulfamethoxazole (SMX) degradation. As synergized by CNTs, the PMS-activation efficiency of MnFeO could be enhanced by>24 times, but with the similar PMS-activation mechanism. It was explored that the SMSI-induced abundant surface hydroxyl groups, in cooperation with the highly hydrophobic CNTs, favored the rapid in situ interfacial degradation of SMX. This feature also endowed the MnFeO-CNTs catalyst resistance to high salinity waters containing inorganic anions (e.g., Cl - and NO 3 – ) of weak complexing abilities. Moreover, the SMSI allowed the greatly accelerated redox cycle rate of Mn species by electron-rich CNTs, resulting in efficient PMS activation. Furthermore, the application feasibility of the MnFeO-CNTs/PMS system was demonstrated for a SMX-spiked real reverse osmosis (RO) concentrate. It was found that higher concentration of PMS could realize the complete removal of SMX, despite the existence of electron-rich tyrosine-like substances would compete with the SMX degradation in the MnFeO-CNTs/PMS system. This study demonstrated that the SMSI could boost the PMS activation , and could serve as an effective material strategy for in situ interfacial organics degradation in the high salinity wastewater.
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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DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Entong Ye,Fangmei Lin,Chengbin Fu,Xin Zhou,Qian Lin,Hongyan Pan,Zheng Chen
A great deal of research has been carried out on the design of Pd-based catalysts in the direct synthesis of H2O2, mainly for the purpose of improving the H2O2 selectivity by weakening the activation energy on the Pd active site and thus inhibiting the dissociation of the O–O bonds in O2*, OOH*, and HOOH*. However, this often results in insufficient activation energy for the reaction between H2 and O2 on Pd, leading to difficulties in improving both the selectivity and productivity of H2O2 simultaneously. Based on this, this study reports an efficient catalyst composed of amine-functionalized SBA-15-supported Pd. The strong metal–support interaction not only makes the PdNPs highly dispersed with more Pd active sites but also improves the stability of the catalyst. The amine group modification increases the proportion of Pd0, further enhancing Pd activity and promoting the adsorption and conversion of H2 and O2 on Pd, thereby significantly increasing H2O2 productivity. Additionally, the density-functional theory simulation results showed that due to the hydrogen-bonding force between the amine group and H2O2, this particular anchoring effect would make the hydrogenation and decomposition of H2O2 effectively suppressed. Ultimately, both the selectivity and productivity of H2O2 are improved simultaneously.
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
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Yunxia Liu,Liang Zhang,Yiming Niu,Bingsen Zhang,Lin Li,Botao Qiao,Junhu Wang
The strong metal-support interaction (SMSI) is able to regulate the electron and geometric structure of supported metal catalysts to improve their performance. However, conventional SMSI formation typically requires high-temperature reduction or oxidation treatments, making it challenging to prevent particle sintering before its establishment. Here, we propose a rapid and energy-efficient microwave treatment to induce SMSI in an Au/CeO 2 system under ambient conditions. Comprehensive characterization confirms that the encapsulation of Au nanoparticles (NPs) and the reduced CO adsorption capacity align with the characteristics of classical SMSI. The rapid generation of oxygen defects and Ce 3+ species in the support is the key to enabling microwave-induced SMSI. As a result, the Au/CeO 2 -MW5 catalysts associated with this SMSI demonstrate excellent stability during a 100-hour test. In addition, this strategy is extendable to various Au-based catalysts supported on metal oxides, such as Au/TiO 2 and Au/ZrO 2 . This work offers an efficient and facile approach to constructing SMSI, potentially laying the foundation for developing encapsulation to enhance the catalyst's stability of noble metal catalysts.
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 Energy Chemistry
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2025
·
IF 14.9
Dexing Li,Zhili Yin,Peixian Wang,Ziqing Wang,Qin Wu,Zhong Wei
Alkaline earth-metal titanates ATiO 3 (A = Ca, Sr, and Ba) with a perovskite-type structure were used as supports for Ru-based catalysts to produce CO x -free H 2 via NH 3 decomposition. The effects of alkaline-earth metals on the physicochemical characteristics and catalytic activities of Ru/ATiO 3 for NH 3 decomposition were investigated using various techniques. The order of Ru/ATiO 3 for NH 3 conversion is Ru/BaTiO 3 > Ru/SrTiO 3 > Ru/CaTiO 3 > Ru/TiO 2 at the identical conditions, with the Ru/BaTiO 3 catalyst demonstrating the highest NH 3 conversion of 77.8% at 450 °C and a gas hourly space velocity of 30,000 mL/g cat /h, which is 8.7, 2.1, and 1.3 times of that over Ru/TiO 2 , Ru/CaTiO 3 , and Ru/SrTiO 3 , respectively. The formation of the ATiO 3 phase can enrich the concentration of basic sites and oxygen vacancies compared with TiO 2 , which can induce the presence of strong metal-support interaction (SMSI) through the formation of Ru–O–Ti bonds. This SMSI effect increased the dispersion and electron density of Ru nano-particles on ATiO 3 supports, and the electron-rich Ru nano-particles could weaken the chemisorptive strength of N 2 and H 2 on the Ru/ATiO 3 catalysts, thereby promoting the reaction rate for NH 3 decomposition.
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
ACTA PHYSICO-CHIMICA SINICA
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2024
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IF 10.8
Hailian Tang,Siyuan Chen,Qiaoyun Liu,Guoyi Bai,Botao Qiao,Fei Liu
The strong metal-support interaction (SMSI) is a widely recognized concept in heterogeneous catalysis, known for significantly enhancing catalyst stability and potentially modulating catalytic performance. However, because the SMSI effect is generally reversible, it tends to diminish under redox conditions opposite to those used for its construction. Consequently, its application is typically limited to conditions that are the same or similar to those under which it was formed. Herein, we report the application of oxidative SMSI (O-SMSI) constructed on hydroxyapatite-supported Rh catalyst (Rh/HAP) in a reductive reaction, the hydrogenation of furfuryl alcohol. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and electron microscopy measurements reveal that high-temperature oxidation treatment at 500 °C induced the occurrence of O-SMSI on the Rh/HAP catalyst, accompanied by the encapsulation of Rh particles by the support. Upon the O-SMSI, the Rh species were effectively stabilized on the support surface, with significant suppression of sintering and leaching during liquid-phase reactions. As a result, the catalyst showed stable furfuryl alcohol conversion and cyclopentanone selectivity during recycling tests. Furthermore, it was found that the O-SMSI and the associated encapsulation behavior on the Rh/HAP system were only partially reversible rather than completely reversible. Even after high-temperature reduction at up to 600 °C, a portion of the SMSI effect remains, ensuring the stability of the catalysts in reductive reactions. This discovery greatly expands the application scope of SMSI catalysts and provides a new way to prepare stable hydrogenation catalysts.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 15
·5059-5066
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IF 9.48
Kaihang Sun,Ning Rui,Zhitao Zhang,Zeyu Sun,Qingfeng Ge,Chang-Jun Liu
Supported Pt catalysts have been extensively investigated for CO2 hydrogenation with methane and CO as the principal products. In this work, a Pt/In2O3 catalyst prepared with decomposition precipitation was tested for CO2 hydrogenation to methanol. The Pt/In2O3 catalyst exhibited a highly improved activity towards CO2 hydrogenation, with methanol selectivity of ca. 100% at temperatures below 225 °C, 74% at 275 °C and 54% at 300 °C, respectively, compared to the pure In2O3 catalyst. This represents the highest methanol selectivity reported on Pt catalysts for CO2 hydrogenation. The stability of the Pt/In2O3 catalyst at elevated temperatures has also been higher than that of the pure In2O3 catalyst, indicated by the methanol formation rate decreasing only to 95% of the initial rate after 5 h in the reaction stream and remaining largely constant thereafter. In contrast, the pure In2O3 catalyst loses 20% of the initial methanol formation rate after 9 h in the reaction stream. The characterization of the catalysts confirms that the Pt nanoparticles are well dispersed on In2O3 with a particle size below 3 nm. The strong metal–support interaction (SMSI) between Pt and In2O3 improves the stability of the catalyst and prevents the over-reduction of In2O3. The synergy between the supported Pt nanoparticles and In2O3 balances the hydrogen activation and the density of the surface oxygen vacancies in In2O3, resulting in the high activity for CO2 hydrogenation and enhanced stability of the Pt/In2O3 catalyst.
研究领域:
催化化学
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能源化学
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材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xiao Chen,Xing-Bao Wang,Shuhua Han,Dong Wang,Chuang Li,Weixiang Guan,Wen-Ying Li,Changhai Liang
Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal–support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO2 supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt–SiO2 interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO2 has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the Pt2Si/SiO2 catalyst with an initial catalytic activity of 2.49 μmol/(m2/g)/h as well as TOF of 0.95 s–1 preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (sym-OHA) by subsequent hydrogenation. In addition, the Pt2Si/SiO2 catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic Pt2Si nanoparticles are anchored firmly onto the surface of the SiO2 support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal–SiO2 interface and tune the surface chemical properties in diverse application conditions.
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
RSC Advances
·
2018
·Vol. 8
·期 31
·17504-17510
·
IF 2.936
Nan Jiang,Xiao Zhou,Yi-Fan Jiang,Zhi-Wei Zhao,Liu-Bo Ma,Cong-Cong Shen,Ya-Nan Liu,Cheng-Zong Yuan,Shafaq Sahar,An-Wu Xu
The design and development of highly efficient and long lifetime Pd-based catalysts for hydrogenation reactions have attracted significant research interest over the past few decades. Rational selection of supports for Pd loadings with strong metal-support interaction (SMSI) is beneficial for boosting catalytic activity and stability. In this context, we have developed a facile approach for uniformly immobilizing ultra-small Pd nanoparticles (NPs) with a clean surface on a Pr6O11 support by a hydrogen thermal reduction method. The hydrogenations of p-nitrophenol and styrene are used as model reactions to evaluate the catalytic efficiency. The results show highly efficient styrene hydrogenation performance under 1 atm H2 at room temperature with a TOF value as high as 8957.7 h−1, and the rate constant value of p-nitrophenol reduction is 0.0191 s−1. Strong metal-support interaction and good dispersion of Pd nanoparticles, as demonstrated by XPS and HRTEM results, contribute to the excellent hydrogenation performance. Electron paramagnetic resonance (EPR) results suggest the presence of oxygen vacancies in the support, which serve as electron donors and enhance the adsorption and activation of reactants and subsequent conversion into products. Moreover, the catalyst can be recovered and reused up to 10 consecutive cycles without marked loss of activity. Overall, our results indicate that oxygen-deficient Pr6O11 nanorods (NRs) not only play a role as support but also work as the promoter to substantially boost the catalytic activities for organic transformations, therefore, providing a novel strategy to develop other high-performance nanostructured catalysts for environmental sustainability.
研究领域:
催化化学
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材料科学
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环境科学
✓ 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）