Small
·
2022
·Vol. 18
·期 45
·2204490
·
IF 15.153
Bing Han,Qinghe Li,Xunzhu Jiang,Yalin Guo,Qike Jiang,Yang Su,Lin Li,Botao Qiao
The switch of CO 2 hydrogenation selectivity from CH 4 to CO over TiO 2 supported Rh catalysts is accomplished via selective encapsulation of Rh nanoparticles while exposing Rh single atoms by high-temperature reduction (HTR) according to their different strong metal-support interaction (SMSI) occurrence conditions, which can be reversed by subsequent oxidation treatment.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Shaodan Xu,Huanxuan Li,Jia Du,Junhong Tang,Liang Wang
We report the synthesis of subnanometric Au clusters with average diameters at 1.2 nm on a low-crystallinity CeO2 support (sub-Au/LC-CeO2), which exhibit high activities and selectivities in the aerobic oxidation of C–H bonds on a series of petroleum-derived hydrocarbons under solvent-free conditions. This phenomenon is strongly related to the maximized strong metal–support interactions between subnanometric Au and the LC-CeO2 support.
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 ELECTRONIC MATERIALS
·
2022
·Vol. 52
·期 1
·342-350
·
IF 2.047
Zheng Cheng,Sun Xueqin,Qin Yanxi,Guo Yan,Yan Jingjing,Tong Xili
The weak interaction between common carbon support and Pt nanoparticles results in low efficiency for the oxygen reduction reaction (ORR) with high overpotentials, which greatly limits the practical application of proton exchange membrane fuel cells. Employing strong metal–support interaction (SMSI) is a promising method for tuning the electronic structure of Pt to boost the ORR, accompanied by rapid improvement in durability. Herein, titanium carbide (TiC) was grown on the surface of carbon black by the sol–gel method coupled with high-temperature treatment (denoted as TiC-C). Based on the SMSI that occurred between TiC and Pt, the obtained Pt/TiC-C catalyst exhibits higher mass ORR activity, which is twice that of the commercial Pt/C-JM under the same conditions. In addition, the Pt/TiC-C exhibits superior durability relative to the Pt/C-JM by preventing the aggregation and dissolution of Pt nanoparticles during the ORR process.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Nano-Micro Letters
·
2021
·Vol. 13
·期 1
·1-13
·
IF 16.419
Chen Keng,Wang Zeming,Wang Liang,Wu Xiuzhen,Hu Bingjie,Liu Zheng,Wu Minghong
High-efficiency electrochemical hydrogen evolution reaction (HER) offers a promising strategy to address energy and environmental crisis. Platinum is the most effective electrocatalyst for the HER. However, challenging scarcity, valuableness, and poor electrochemical stability still hinder its wide application. Here, we designed an outstanding HER electrocatalyst, highly dispersed rhodium (Rh) nanoparticles with an average diameter of only 3 nm supported on boron (B) nanosheets. The HER catalytic activity is even comparable to that of commercial platinum catalysts, with an overpotential of only 66 mV in 0.5 M H 2 SO 4 and 101 mV in 1 M KOH to reach the current density of 10 mA cm −2 . Meanwhile, the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media, even the simulated seawater environment. Theoretical calculations unraveled that the structure–activity relationship between B(104) crystal plane and Rh(111) crystal plane is beneficial to the release of hydrogen, and surface O plays a vital role in the catalysis process. Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Guanfeng Tian,Youqing Wu,Shiyong Wu,Sheng Huang,Jinsheng Gao
Synthesizing methanol from CO 2 and green hydrogen is a promising strategy to solve environmental issues and meet the increasing energy demand. In this work, Pd/MnO/In 2 O 3 catalyst with highly dispersed Pd species was prepared via an in-situ reduction method using NaBH 4 as the reducing agent. The highly dispersed Pd species promoted the dissociative of hydrogen and the hydride species could spill over to the MnO/In 2 O 3 due to the strong metal-support interaction between Pd and MnO/In 2 O 3 , which improved the catalytic activity of Pd/MnO/In 2 O 3 for CO 2 hydrogenation to methanol. As a result, the methanol space-time yield of 1 wt% Pd/MnO/In 2 O 3 was 4.8 times higher than that of MnO/In 2 O 3 . Moreover, the methanol selectivity of 1 wt% Pd/MnO/In 2 O 3 was still higher than 70% at a temperature below 280 °C. The present in-situ reduction method is an effective route for the preparation of Pd/MnO/In 2 O 3 catalyst for CO2 hydrogenation to methanol.
研究领域:
催化化学
·
环境科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Xiaoyan Liu,Yiqi Ren,Maodi Wang,Xiaomin Ren,Jian Liu,Qihua Yang
Selective hydrogenation of nitrobenzothiazole to aminobenzothiazole with metal catalysts is an economical process for the synthesis of pivotal intermediates for thiazole drugs, but it is still very difficult due to the easy deactivation of metal catalysts by sulfur-containing compounds. Herein, we report efficient nitrobenzothiazole hydrogenation using Pt/TiO2 as a catalyst. Pt/TiO2 with the strong metal–support interaction (SMSI) effect was found to be more active than Pt/TiO2 without the SMSI effect. Density functional theory (DFT) calculations and S-resistance experiments revealed that the −NO2 group is activated mainly by the oxygen vacancy (Ov) of TiOx in the presence of sulfur compounds and that H species dissociated on Pt spills over to reduce −NO2. The high nitrobenzothiazole hydrogenation activity of Pt/TiO2 can be attributed to a cooperative effect between Pt and TiOx. The generation of SMSI not only induces more Ov sites but also enhances the H-spillover capability. This study provides deep insight into the development of highly efficient platinum-S resistance hydrogenation 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 COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xin Deng,Jingyi Chen,Chenyang Zhang,Yong Yan,Bingzheng Wu,Jie Zhang,Gang Wang,Ruilin Wang,Jinwei Chen
Catalysts for the electrolysis of water are critical in the production of hydrogen for the energy industry. The use of strong metal-support interactions (SMSI) to modulate the dispersion, electron distribution, and geometry of active metals is an effective strategy for improving catalytic performance. However, in currently used catalysts, the supporting effect does not significantly contribute directly to catalytic activity. Consequently, the continued investigation of SMSI, using active metals to stimulate the supporting effect for catalytic activity, remains very challenging. Herein, the atomic layer deposition technique was employed to prepare an efficient catalyst composed of platinum nanoparticles (Pt NPs) deposited on nickel-molybdate (NiMoO 4 ) nanorods. Nickel-molybdate’s oxygen vacancies (V o ) not only help anchor highly-dispersed Pt NPs with low loading but also strengthen the SMSI. The valuable electronic structure modulation between Pt NPs and V o resulted in a low overpotential of the hydrogen and oxygen evolution reactions, returning results of 190 mV and 296 mV, respectively, at a current density of 100 mA cm −2 in 1 M KOH. Ultimately, an ultralow potential (1.515 V) for the overall decomposition of water was achieved at 10 mA cm −2 , outperforming state-of-art catalysts based on the Pt/C || IrO 2 couple (1.668 V). This work aims to provide reference and a concept for the design of bifunctional catalysts that apply the SMSI effect to achieve a simultaneous catalytic effect from the metal and its support.
研究领域:
材料科学
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催化化学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Songshan Zhu,Shimin Ma,Di Song,Yunzhu Wang,Jichang Lu,Tianhao Ai,Huihui Lu,Sufang He,Yongming Luo
The dynamic relationship of TiO 2 crystal phase and strong metal-support interactions (SMSI) of Ni/TiO 2 catalyst was investigated to reveal the induction period of glycerol steam reforming. Comprehensive investigations confirmed that the SMSI between Ni 0 and anatase TiO 2 was formed by anatase TiO 2 encapsulated Ni 0 after H 2 reduction at 500 °C for the Ni/TiO 2 catalyst calcined at 500 °C (Ni/Ti-500R), which inhibited the contact of Ni 0 active sites with reactants and led to the low hydrogen yield in the initial stage of the reaction. Interestingly, the dynamic conversion of anatase to rutile during the GSR process at 600 °C caused the TiO 2 overlayers on the Ni 0 particles to gradually fade, exposing more Ni 0 sites, resulting in a gradual increase in hydrogen yield to 5.93 mol H2 /mol glycerol . In addition, Ni/Ti-500R with a dynamic SMSI inhibited Ni 0 particles sintering and encapsulated carbon deposition, resulting in relatively better stability (21 h) after induction period. In comparison, the designed Ni/TiO 2 catalyst calcined at 600 °C (Ni/Ti-600R) with rutile TiO 2 as the main component inhibited the formation of the classical SMSI, even after 600 °C H 2 reduction, and no excessive TiO 2 encapsulated Ni 0 particles were observed, so no obvious induction period occurred. This study provides new insights into the relationship of SMSI with crystal phases and the induction period in multiphase catalysis, also a new strategy for designing efficient 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
Nano Energy
·
2024
·
IF 16.8
Jiarun Cheng,Chaojie Lyu,Hang Lei,Xueyan Li,Hongyue Zhu,Dan Zhou,Wenjie Mai,Yiming Liu
The regulatory mechanism of strong metal-support interaction (SMSI) is of great significance in improving the electrocatalytic performance for supported electrocatalysts. Here, PtNi alloy nanoparticles were deposited on N, F-codoped graphene-like carbon nanosheets (PtNi@NFGC) to construct a highly active interface for efficient methanol oxidation reaction (MOR), which solves the problems of high cost, poor activity and easy aggregation of Pt-based catalysts. Due to the high electrophilicity, F atoms doping into the carbon lattice can not only manipulate the electron structure and the state of the carbon skeleton, but also further trigger the stronger charge transfer between metal atoms and carbon support. Compared with single-doped PtNi@NGC, N, F-codoped PtNi@NFGC possesses a lower onset potential and methanol oxidation potential, higher methanol oxidation current and stronger CO tolerance. The results of the partial density of state (PDOS) simulation display that N, F-codoping promotes the electron transfer from Pt atoms to NFGC support, and leads to the d-band center shift upward, thus strengthening the oxidation degree of Pt active sites and increasing the composition of high-valent Pt x+ . In-situ Raman analysis and density functional theory (DFT) results expound that F atoms embedding observably enhances the adsorption energy of Pt active centers to *OH intermediates, which not only significantly improves MOR catalytic activity, but also achieves efficient methanol dehydrogenation and alleviates CO poisoning. This customization of metal-support interface interaction by heteroatom doping strategy opens up opportunities for designing efficient supported catalysts.
研究领域:
电化学
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2022
·Vol. 95
·期 5
·759-767
·
IF 5.121
Cao Pengfei,Zhao Haitao,Adegbite Stephen,Lester Edward,Wu Tao
In this study, a co-precipitation coupled with vacuum-freeze drying (VFD) method was adopted to fabricate a highly mesoporous nickel-aluminium catalyst (VFD-cat). VFD-cat with uniform smaller pore size and a larger BET surface area were obtained than the catalysts prepared following the conventional thermal evaporation drying method (TED-cat). In addition, the VFD method helps to improve the dispersion of precursors, which then enhances the strong metal-support interactions (MSI) of VFD-cat via forming substoichiometric NiAl2O4 spinel. Characterization showed that the average nickel particle size on the VFD-cat was smaller than that of the TED-cat, attributed to the confinement effects of MSI. At 800 °C, the VFD-cat exhibited higher stability during the long-term dry reforming of methane (DRM) test. It was found that the coke formation on spent VFD-cat, especially for the ordered carbon species, was significantly eliminated as compared with TED-cat after the stability test. This strategy offers a facile way to develop DRM catalysts with highly mesoporous and MSI, enhancing the catalytic stability and coke resistance of the nickel-aluminium catalyst.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Nanzhu Nie,Dan Zhang,Zuochao Wang,Shijie Ge,Yanli Gu,Bo Yang,Jianping Lai,Lei Wang
Achieving acidic seawater hydrogen production under commercial current densities remains a challenge. We present here a novel strategy through strong metal-support interaction (SMSI) and Pt-p-block alloys (PtM@CNT, M = Ga, In, Pb, and Bi) to construct a stable electronic perturbation and achieve acidic seawater hydrogen evolution performance at commercial current densities for the first time. SMSI stabilizes electronic perturbation and promotes durability up to 360 h. The optimized Pt 61 Ga 39 @CNT exhibits an overpotential of 18 mV at 10 mA cm −2 in 0.5 M H 2 SO 4 and maintains 360 h stability at 500 mA cm −2 in acidic seawater. Density functional theory (DFT) calculation reveals that the optimized d -band center of Pt and ΔG H* increase the catalytic activity, and the higher vacancy formation energy enhances the durability. Overall, this discovery not only first achieves stable acidic seawater hydrogen production under commercial current densities, but also opens a new opportunity to explore catalytic applications of p-block alloys and SMSI stabilized electronic perturbation.
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
危险品化学品经营许可证（带存储）