NANOTECHNOLOGY
·
2024
·
IF 2.9
Xinbiao Mao,Mingyu Ou,Wenjun Zhao,Meiqin Shi,Lingxia Zheng
It is a challenge to improve the long-term durability of Pd-based electrocatalysts for oxygen reduction reaction (ORR) in fuel cells. Herein, Pd/CeO2-C-T (T=800, 900 and 1000℃) hybrid catalysts with metal-support interaction are prepared from Ce-based metal organic framework (Ce-MOF) precursor. Abundant tiny CeO2 nanoclusters are produced to form nanorod structures with uniformly distributed carbon through a calcination process. Meanwhile, both carbon and CeO2 nanoclusters have good contact with the following deposited surfactant-free Pd nanoclusters. Benefited from the large specific surface area, good conductivity and structure integrity, Pd/CeO2-C-900 exhibits the best electrocatalytic ORR performance: onset potential of 0.968 V and half-wave potential of 0.857 V, outperforming those obtained on Pd/C counterpart. In addition, the half-wave potential only shifts 7 mV after 6000 cycles of accelerated durability testing, demonstrating robust durability.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
HELVETICA CHIMICA ACTA
·
2023
·Vol. 106
·期 5
·e202200203
·
IF 1.8
Peng Liu,Xin Zhang,Yuan-Yuan Huang,Geng-Wei Liu,Chen-Jie Li,Pin-Mei Yan,Ye-Yan Qin,Rong Guo,Si-Qi Wu,Yun-Yun Zeng,Peng-Bin Pan,Yuan-Gen Yao
High active Pd-based catalyst with low loading capacity for CO oxidative coupling with methyl nitrite (MN) to dimethyl oxalate (DMO) has aroused great interest in the large-scale production of DMO for the next hydrogenation to bring forth ethylene glycol (EG). Here, spinel composite oxide support, namely MgAl 2 O 4 , had been prepared through three different methods: solid combustion method (MAO-SC), hydrothermal method (MAO-HT) and co-precipitation method (MAO-CP), and further Pd nanoparticles were anchored to the surface of MgAl 2 O 4 through a simple wetness impregnation method. In the CO direct esterification to DMO reaction, the Pd/MAO-SC catalyst, which used MgAl 2 O 4 support prepared by solid combustion method, exhibited the highest intrinsic activity with Turnover frequency (TOF) value of 2.39 s −1 and DMO weight space-time yield (956.8 g⋅kg cat −1 ⋅h −1 ) with 44.1 % CO conversion and 97.8 % DMO selectivity, and showed negligible attenuation of activity during the process of continuous reaction for 100 h. The characterization results confirmed that abundant oxygen defect sites occurred in MAO-SC synthesized by combustion method not only can help to anchor the Pd nanoparticles with appropriate size and dispersion, but also can promote the interfacial electron transfer from MgAl 2 O 4 support to Pd nanoparticles, thus significantly enhancing the metal-support interaction (MSI) and providing more CO bridge-adsorption sites that is favorable for the CO oxidative coupling with MN to DMO reaction.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Yixuan Wang,Hongyan Ban,Yugao Wang,Ruwei Yao,Shimin Zhao,Jiangliang Hu,Congming Li
Basic sites profoundly affect the mode and strength of CO 2 adsorption in the hydrogenation of CO 2 to formic acid (FA), however, the mechanism by which the quantities and strength of basic sites affect the reaction process is not yet clear. Herein, a Ni/Mg a AlO x catalyst has been developed and the basic sites of the catalyst can be modulated by simply altering the Mg/Al ratio. Through a series of characterizations and experiments, it was observed that weak and medium basic sites synergistically catalyzed the hydrogenation of CO 2 to formic acid, and a reasonable number of weak basic sites can improve reaction performance when a sufficient number of medium basic sites guarantee the fundamental catalytic activity. Moreover, the number and distribution of basic sites are also tightly related to metal-support interactions. This strategy provides theoretical guidance and a feasible scheme for optimizing the performance of non-precious metal heterogeneous catalysts.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Guangping Zhou,Hao Huang,Bo Yang,Xuan Zhou,Huoyan Jiang,Da Zhang,Wanli Zhang,Shaoqu Xie
A carbon-doped Cu/Al 2 O 3 catalyst was engineered using glucose, fructose, and sucrose as carbon sources. Controlled carbon deposition and calcination exposed acidic sites, thereby optimizing Cu dispersion, enhancing metal–support interaction (SMSI), and enriching surface hydroxyls, which collectively facilitated CO 2 hydrogenation via HCOO ∗ and ethyl acetate intermediates. Structural characterization showed that the preferential exposure of the Cu (111) crystal face further enhanced the catalytic activity. Performance tests showed that the catalyst exhibited a methanol yield of 12 % and a selectivity of 91 % in the CO 2 hydrogenation to methanol reaction, which was attributed to the improved Cu dispersion, the enriched metal Cu phase, and the presence of acidic sites. This study provides new ideas for the rational design of Cu-based catalysts and proposes a scalable green synthesis method for methanol.
研究领域:
催化化学
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材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2024
·
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
Chemistry-An Asian Journal
·
2018
·Vol. 13
·期 6
·641-647
·
IF 3.692
Lifang Xie,Ting Chen,Hang Cheong Chan,Yijin Shu,Qingsheng Gao
Graphical The straight dope : Controlled hydrogen doping into MoO 3 supports by means of H 2 spillover was introduced to vary the metal–support interactions with Ir, thereby achieving efficient hydrogenation of furfural to furfuryl alcohol under mild conditions (see figure). As promising supports, reducible metal oxides afford strong metal–support interactions to achieve efficient catalysis, which relies on their band states and surface stoichiometry. In this study, in situ and controlled hydrogen doping (H doping) by means of H 2 spillover was employed to engineer the metal–support interactions in hydrogenated MoO x -supported Ir (Ir/H−MoO x ) catalysts and thus promote furfural hydrogenation to furfuryl alcohol. By easily varying the reduction temperature, the resulting H doping in a controlled manner tailors low-valence Mo species (Mo 5+ and Mo 4+ ) on H−MoO x supports, thereby promoting charge redistribution on Ir and H−MoO x interfaces. This further leads to clear differences in H 2 chemisorption on Ir, which illustrates its potential for catalytic hydrogenation. As expected, the optimal Ir/H−MoO x with controlled H doping afforded high activity (turnover frequency: 4.62 min −1 ) and selectivity (>99 %) in furfural hydrogenation under mild conditions ( T= 30 °C, P =2 MPa), which means it performs among the best of current catalysts.
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
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 15
·5059-5066
·
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
·
能源化学
·
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
·
材料科学
✓ 已验证
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
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jie Fan,Yuhang Sun,Mingli Fu,Jiaqi Li,Daiqi Ye
Metal support interactions modulation is one of the effective strategies to enhance the catalytic performance. Herein, we reported that modulating metal support interactions by switching the strength (CO, H 2 , NH 3 ) and temperature (200, 300, 400 °C) of reducing gases is a facile way to improve the catalytic performance of Pt/CeO 2 for toluene oxidation . The distinct reduction treatments will stepwise enhance the reducibility, ratio of Pt 0 and oxygen vacancy concentration, which dominated the activity. The metal support interactions modulation can significantly affect toluene deep oxidation (from benzoate to formate or monodentate carbonate) via enhancing the mobility of surface/lattice oxygen and activation ability towards O 2 molecules, since the main activation sites for O 2 molecules expand from Pt 0 sites to oxygen vacancies and Pt 0 sites with temperature increasing.
研究领域:
催化化学
·
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）