Catalysts
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2022
·Vol. 12
·期 5
·527
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IF 4.501
Zihao Li,Xianhuai Chen,Jinghuan Chen,Huazhen Chang,Lei Ma,Naiqiang Yan
Nowadays, the oxidation activity at the low-temperature regime for Co3O4catalysts needs to be improved to meet the stringent regulation of multi-pollutant diesel exhaust. Herein, nanoflower-like Co3O4diesel oxide catalysts (DOCs) were fabricated with the addition of a low-content Pt to trigger better catalytic activities for oxidizing multi-pollutants (CO, C3H6, and NO) emissions by taking advantage of the strong-metal supporting interaction. Compared to the conventional DOCs based on Pt/Al2O3, the as-synthesized Pt/Co3O4catalysts not only exhibited better multi-pollutants oxidation activities at the low temperature but also obtained better resistance toward NO inhibition. Moreover, Pt/Co3O4catalysts showed exceptional hydrothermal durability throughout long-term tests in the presence of water vapor. According to the XPS and H2-TPR results, Pt promoted low-temperature catalytic activity by increasing the active surface oxygen species and reducibility due to the robust synergistic interaction between metallic Pt and supporting Co3O4. Meanwhile, TGA curves confirmed the Pt atoms that facilitated the desorption of surface-active oxygen and hydroxyl radicals in a low-temperature regime. Furthermore, instead of probing the intermediates during CO and C3H6oxidation for Pt/Co3O4catalysts, which included carbonates, formate, and acetate species, in situ DRIFTs experiments also revealed C3H6oxidation mainly took place over metallic Pt sites.Keywords:diesel oxide catalysts;catalytic oxidation;strong metal–support interaction;cobalt oxides;platinum
研究领域:
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yimin Zhang,Yun Zu,Dedong He,Jun Liang,Linhua Zhu,Yi Mei,Yongming Luo
Strong metal support interaction between Ni and γ-Al 2 O 3 , resulted from the excessive hydroxyl groups on the Al 2 O 3 support, has restricted Ni utilization in the traditional Ni/Al 2 O 3 catalyst, which hampered its commercial application. Meanwhile, the concept of surface defects in activating single-carbon chemicals of CH 4 and CO 2 has attracted much attention in heterogeneous catalysis. Thus, designing better Ni/Al 2 O 3 system in generating surface defects without losing active Ni into Al 2 O 3 support remains challenging. Herein, the development of tailored defect sites on Al 2 O 3 through hydroxyl-exposed strategy shows dual role of stabilizing the active Ni sites and holding responsible for catalyzing CH 4 dry reforming (DRM) reaction via a more efficient route, which emphasizes the superior behavior of the traditional Ni/Al 2 O 3 catalyst. It is considered that it can be appropriately used for reactions using not only excellent DRM catalysts but also other Ni catalysts.
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
JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Akihiro Nakayama,Ryusei Sodenaga,Yuvaraj Gangarajula,Ayako Taketoshi,Toru Murayama,Tetsuo Honma,Norihito Sakaguchi,Tetsuya Shimada,Shinsuke Takagi,Masatake Haruta,Botao Qiao,Junhu Wang,Tamao Ishida
Cation- and anion-substituted hydroxyapatites (sHAPs) supported gold catalysts showed strong metal-support interaction (SMSI) under oxidative atmosphere. Mg- and Ce-substituted sHAPs stabilized Au clusters and imparted positively charged Au. The Au on these sHAPs became more positively charged upon formation of the oxidative SMSI. The catalytic activities for transvinylation of benzoic acid with vinyl acetate and isomerization of 3,4-diacetoxybut-1-ene (34DABE) correlated well with the cationic properties of Au; Au/Mg0.1SrHAP and Au/Ce0.1SrHAP with SMSI exhibited higher catalytic activity than other Au/sHAPs and the same catalysts without SMSI. The enhanced cationic properties of Au particles induced by oxidative SMSI surpassed the disadvantages of the reduction of the exposed surface Au atoms caused by SMSI. This work reveals that controlling the degree of SMSI is an efficient methodology to tune an optimal electronic state of metal NPs for target reactions and to provide highly active and durable catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Hua Yang,Ruofan Yu,Yuan Fang,Jikang Yao,Yuyan Gan,Jian Chen,Hongtao Deng,Xinhua Gao,Xupeng Zong,Jinming Wang,Lizhi Wu,Li Tan,Yu Tang
The interaction between metal and support is an essential topic in heterogeneous catalysis. The role of strong metal-support interaction (SMSI) between support and metal particles, oxide, or single atom site in catalysis has been investigated recently. In this work, we report a singly dispersed bimetallic site (SDBM), Ir 1 Ti 3 , formed on TiO 2 support during partial oxidation of methane. The Ir 1 Ti 3 site exhibits an unusual “switch on/off” catalytic activity for partial oxidation of methane to produce syngas, which is due to the strong interaction between TiO 2 support and in-situ formed Ir 1 Ti 3 SDBM site. The high activity and stability of the catalyst are also due to the unique structure according to the strong interaction effect. This work reveals the SMSI between oxide and SDBM and further impacts on catalysis.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wei Liu,Hui Sheng,Liu Zhu,Yiwen Zhang,Wenxu Liu,Yuwei Zhao,Qian Li,Yong Peng,Zhongpeng Wang
The classical strong metal-support interaction (SMSI) plays a key role in improving thermal stability for supported Au catalysts. However, it always decreases the catalytic activity because of the encapsulation of Au species by support. Herein, we demonstrate that Al 3+ is a functional additive which could effectively improve both catalytic activity and sintering resistant property for H 2 pretreated Al 3+ doped CeO 2 supported Au (AuCeAl) catalyst at high temperature. The physical characterization and in-situ DRIFTS results provide insight that more oxygen vacancies generated by Al 3+ doping could be as preferential adsorption sites for CO molecules when the encapsulation of Au species occurred, which is certificated by an accelerated formation of bicarbonate species. In the meantime, smaller Au nanoparticles with higher dispersion (2.8 nm, 85.63%) is achieved in AuCeAl catalysts, compared with that in CeO 2 supported Au (AuCe) catalysts (5.1 nm, 36.17%). Additionally, the as-prepared AuCeAl catalysts also have superior catalytic performance even after calcination at 800 °C in air.
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
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 15
·8248-8255
·
IF 11.9
Liang Shen,Wenhao Zhang,Yifei Feng,Jing Xu,Minghui Zhu
Hydrogenation of CO2 to produce high-value chemicals is a response to increasing environmental and energy concerns. The target products of CO2 hydrogenation, methane and CO, are both important energy sources and raw materials for the production of higher hydrocarbons. Therefore, it is very important to understand the mechanism of selectivity control of catalysts. In this work, we aim to elucidate the selectivity regulation of Zn on Ni catalysts, which has been extensively studied in the literature without reaching a consensus. We have prepared a series of catalysts with different Zn content and systematically investigated the relationship between their structural evolution and selectivity. It is found that the introduction of Zn preferentially forms an alloy with Ni and at higher loadings is present as ZnOx, which participates in the strong metal–support interaction (SMSI). The conversion of the active sites into a Ni–Zn alloy hinders further hydrogenation of the adsorbed CO intermediates and makes the catalyst CO-selective. The presence of the Ni–ZnOx interface changes the CO2 activation mechanism from an association pathway to a redox pathway.
研究领域:
催化化学
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能源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Chengbin Wang,Ping Li,Lingbo Zong,Kaicai Fan,Fenghong Lu,Zumin Wang,Lei Wang
Developing cost effective, active and durable alternatives to platinum electrocatalysts is the major challenge for sustainable hydrogen production. Rational design and controlled synthesis of hybrid structures with strong metal-support interaction may offer a feasible strategy to achieve efficient and stable hydrogen evolution reaction (HER). Herein, a low cost and high-performance ultrafine Ru nanoparticles anchored tungsten carbide ( Ru/WC) HER electrocatalyst is successfully prepared by high-temperature shock (HTS) technology, which can be accomplished in less than 0.5 s. In a strong alkaline medium, the as-prepared Ru/WC exhibits a low overpotential of 4 mV and 72 mV at the current densities of 10 mA cm −2 and 100 mA cm −2 , respectively. Low Tafel slope of 44 mV dec −1 , high turnover frequency (TOF) of 2.55 s −1 at an overpotential of 100 mV, long-term electrochemical stability up to 150 h, and ampere-level current density can be achieved. Furthermore, Ru/WC also shows exceptional activity and stability under acidic conditions. Notably, Ru/WC can accommodate HER current density as high as 2000 mA cm −2 at a small overpotential of 365 mV, which holds great promises for industrial large-scale production. This work provides a simple, rapid, and solvent-free strategy for synthesizing high efficiency HER electrocatalyst with ampere-level current density.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Fangxu Lu,Song Wen,Jie Jiang,Jinchong Zhao,Changsheng Zhang,Junjie Feng,Jing Zhang,Bing Sun,Wei Xu
It is generally acknowledged that the crystal structure of the support plays a crucial role in the catalytic performance, however, the exact role of crystal structure in the catalytic system remains controversial. The Pd/TiO2 catalysts designed in this study with different crystals (rutile (r) and anatase (a)) were employed to study the effects of the crystal structure via a probe reaction for oxygen removal under a hydrogen atmosphere. Under the same reaction conditions, the temperature to achieve 90% O2 conversion on Pd/a-TiO2 could reach up to 150 °C, which is ∼1.4 times (107 °C) that of the Pd/r-TiO2 catalyst. Based on the various characterization results, it is found that strong metal support interactions (SMSIs) are dominant on the Pd/r-TiO2 catalyst, which could facilitate the formation of oxygen vacancies and Pd2+ species in the active sites, resulting in excellent catalytic performance. This study not only improves the understanding of the distinctive structural properties of TiO2 crystal support but also offers an effective strategy to design efficient heterogeneous catalysts via tuning SMSIs.
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
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Zijiang Zhao,Songtao Huang,Guanglu Dong,Yi Chen,Mingxuan Wang,Molin Xia,Xin Song,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
The hydrogenation of vanillin stands as a pivotal platform reaction within biomass conversion processes, presenting a significant challenge in achieving controlled synthesis of different products. Here, we proffer different methodology for elaborately designing the electronic structure of Pt via regulating the strong metal-support interactions (SMSI) between Pt and Mo 2 TiC 2 , thereby facilitating the targeted synthesis of vanillyl alcohol (VA) and 2-methoxy-4-methylphenol (MMP) from vanillin. Appropriate H 2 reduction can enhance the SMSI between Pt and Mo 2 TiC 2 , promoting the electron transfer from Mo 2 TiC 2 to Pt, resulting in 200-Pt/Mo 2 TiC 2 with 68.1 of Pt 2+ . However, the SR-Pt/Mo 2 TiC 2 obtained through the galvanic replacement strategy possesses 64.7 % of Pt 4+ , which is attributed to the weaker spontaneous SMSI between Pt and Mo 2 TiC 2 . XPS adsorption experiments highlight the pivotal role of Pt 2+ in facilitating the desorption of VA, resulting in the 200-Pt/Mo 2 TiC 2 catalyst demonstrating exceptional selectivity towards VA (96 %). Meanwhile, SR-Pt/Mo 2 TiC 2 showcases a predilection for the direct hydrogenation and deoxygenation of vanillin into MMP. This research not only marks the application of the MXene system to biomass conversion but also illuminates the relationship between the electronic structure of Pt and its selectivity towards VA and MMP.
研究领域:
化学工程
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催化
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Yulu Chen,Hongyan Pan,Chunliang Yang,Haipeng Xiao,Zheng Chen,Chun Zhu,Weiyue Zhao,Qian Lin
Direct synthesis of hydrogen peroxide (H2O2) by hydrogen and oxygen is an atom-efficient and environmentally benign method. However, achieving high H2O2 selectivity and productivity with sub-nanometer Pd clusters remains challenging due to the tendency of undercoordinated surface sites to cleave O-O bonds and form water. Herein, sub-nanometer Pd clusters are confined to ammonia-treated ZIF-8-derived mesoporous carbon (ZDC) with controlled nitrogen configurations, which facilitates the effective direct synthesis of H2O2 by optimizing the electronic structure of Pd atoms via strong metal-support interaction (SMSI). The sub-nanometer catalyst Pd/ZDC1.0 achieves a remarkable H2O2 selectivity of 81.6% and productivity of 3317 mmol/gPd•h-1, which is 12.5% and 123.1% higher than the sub-nanometer catalyst Pd/XC-72 without nitrogen doping, respectively. Structural characterization shows that the pore structure and pyridine nitrogen content of Pd/ ZDCX are proportional to the ammonia-treated time. Theoretical calculations demonstrate that there is a strong electron transfer between sub-nanometer Pd clusters and pyridine nitrogen sites, leading to a downward shift in the d-band center of Pd atoms. The electronic effect weakens the adsorption of reactive intermediates on undercoordinated surface sites and suppresses O-O bond dissociation, contributing to enhanced selectivity and preventing water formation
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
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Qijun Pei,Teng He,Yang Yu,Zijun Jing,Jianping Guo,Lin Liu,Zhitao Xiong,Ping Chen
The strong metal–support interaction (SMSI) is of significant importance to heterogeneous catalysis. The electronic modification and encapsulation of active metals by reducible supports are the intrinsic properties of the SMSI, where the latter would decrease or even cease the catalytic activity of transition metals. Here, we demonstrate for the first time that alkalies are the functional additives that can effectively manipulate the SMSI for better hydrogenation catalysis. Specifically, both thermodynamic analyses and experimental results show that the addition of alkalies to the Ru/TiO2 catalyst could form a titanate top layer that effectively hampers the migration of TiO2–x to the surface of Ru nanoparticles. In the meantime, a substantially enhanced reduction of the support is achieved, leading to an even stronger electron donation from the support to Ru. The alkali-modified Ru/TiO2 exhibits superior low-temperature catalytic activity in the hydrogenation of aromatics, which is ca. an order of magnitude higher than that of the commercial Ru/Al2O3 catalyst and is in clear contrast to that of the neat Ru/TiO2 catalyst that shows negligible activity due to the severe encapsulation of Ru by TiO2–x.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2020
·
IF 4.189
Ting Wang,Xueqin Tao,Donghai Wu,Xiaoying Lu,Qian Yu,Shoujie Liu,Houyang Chen,Benxia Li
Heterogeneous Pd-based catalysts are receiving great attention in cross-coupling reactions due to their distinct advantages of relatively low cost, high stability, easy separation, and recycling. Nonetheless, great challenges still remain in developing heterogeneous catalysts with excellent performance and revealing the origin for efficient catalysis. Herein, we have synthesized a PdOx/NiO NFs catalyst consisting of porous NiO nanofibers and in situ anchored PdOx species by a facile electrospinning–pyrolysis strategy. The electron transfer from NiO to PdO created during the calcination step results in the formation of Pdδ+ (δ < 2) in the PdOx/NiO NFs, validated by both spectroscopic analyses and computational modeling. The PdOx/NiO NFs catalyst exhibits much higher activity than the commercial 5.0 wt % Pd/C and other as-prepared Pd-based catalysts in Suzuki coupling reactions. The turnover frequency (TOF) values for the conversions of iodo-, bromo-, and chlorobenzenes over the PdOx/NiO NFs catalyst are 6.6–7.3 times those over the commercial 5 wt % Pd/C catalyst. Theoretical calculations demonstrate that the configuration of PdO(101)/NiO(111) surface is more propitious to the adsorption and activation of arylhalide and phenylboronic acid than that of Pd(111)/NiO(111) surface. The compelling performance of PdOx/NiO NFs is mainly attributed to the special surface configuration of PdOx and unique electronic state of Pdδ+ species. These traits can be well retained in a long-term reaction owing to the strong metal–support interaction, ensuring the good durability of the catalyst. This study not only develops a promising heterogeneous catalyst with high performance for green synthesis of fine chemicals but also provides insights into the enhancement of catalytic activity achieved by modulating the active centers.
研究领域:
催化化学
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材料科学
·
理论计算化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）