Journal of Environmental Sciences
·
2022
·
IF 6.796
Wei Shi,Guangyan Xu,Xuewang Han,Yingjie Wang,Zhi Liu,Sen Xue,Nannan Sun,Xiaoyan Shi,Yunbo Yu,Hong He
Pd/Al 2 O 3 catalysts supported on Al 2 O 3 of different particle sizes were synthesized and applied in methane combustion. These catalysts were systematically characterized by Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), high resolution-transmission electron microscopy (HR-TEM), high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), H 2 -temperature-programmed reduction (H 2 -TPR), O 2 -temperature-programmed oxidation (O 2 -TPO), X-ray photoelectron spectroscopy (XPS), and X-ray absorption fine structure (XAFS). The characterization results indicated that nano-sized Al 2 O 3 enabled the uniform dispersion of palladium nanoparticles , thus contributing to the excellent catalytic performance of these nano-sized Pd/Al 2 O 3 catalysts. Among them, Pd/Al 2 O 3 -nano-10 (Pd/Al 2 O 3 supported by alumina with an average particle size of 10 nm) showed superior catalytic activity and stability for methane oxidation under harsh practical conditions. It maintained excellent catalytic performance for methane oxidation for 50 hr and remained stable even after harsh hydrothermal aging in 10 vol.% steam at 800°C for 16 hr. Characterization results revealed that the strong metal-support interactions and physical barriers provided by Al 2 O 3 -nano-10 suppressed the coalescence ripening of palladium species, and thus contributed to the superior sintering resistance of the Pd/Al 2 O 3 -nano-10 catalyst.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
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IF 9.9
Huihui Shi,Peixin Yang,Lu Huang,Yali Wu,Duohuan Yu,Hangfei Wu,Yunhuai Zhang,Peng Xiao
The design and manufacture of high activity and thermal stability catalysts with minimal precious metal loading is essential for deep degradation of volatile organic compounds (VOCs). In this paper, a novel single-atom Pt-CeO 2 /Co 3 O 4 catalyst with ultra-low Pt loading capacity (0.06 wt%, denoted as 0.06Pt-SA) was fabricated via one-step co-precipitation method. The 0.06Pt-SA exhibited excellent toluene degradation activity of T 90 = 169 °C, matched with the nanoparticle Pt-supported CeO 2 /Co 3 O 4 catalyst with more than six times higher Pt loading (0.41 wt%, denoted as 0.41Pt-NP). Moreover, the ultra-long durability (toluene conversion remains 99% after 120 h stability test) and excellent toluene degradation ability in a wide space speed range of 0.06Pt-SA were superior to that of 0.41Pt-NP catalyst. The excellent performance was derived from the strong metal-support interaction (SMSI) between the single atomic Pt and the carrier, which induced more Pt 0 and Ce 3+ for oxygen activation and more Co 3+ for toluene removal. The in situ diffuse reflectance infrared spectroscopy (DRIFTS) experiments confirmed that the conversion of intermediates was accelerated in the reaction process, thereby promoting the toluene degradation. Our results should inspire the exploitation of noble single-atomic modification strategy for developing the low cost and high performance VOCs catalyst.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
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IF 11.698
Yazhi Yin,Bing Hu,Xinliang Li,Xiaohai Zhou,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to methanol provides a means of CO 2 fixation and a way of hydrogen storage in a more energy-dense and transportable form. Pd-ZnO catalysts can be active for this reaction, but their activities are strongly associated with the preparation methods which influence the dispersion and stability of Pd nanoparticle. Here we report a novel fabrication of highly effective PdZn alloy catalysts derived from Pd@zeolitic imidazolate framework (ZIF-8) for the hydrogenation of CO 2 . The confinement of subnanometric Pd particles in the pore framework of ZIF-8 facilitates the formation of Pd-ZnO interfaces with strong-metal-support-interaction (SMSI) after a simple pyrolysis under air condition. The porous texture and high surface area of ZnO ensures a high dispersion of Pd nanoparticles. Different pyrolysis temperatures were studied in catalysis and the highest methanol yield reached 0.65 g g cat −1 h −1 at 270 °C, 4.5 MPa, with a TOF of 972 h −1 , over a PdZn catalyst prepared at 400 °C. Such excellent activity has ranked the top reported values over advanced Pd-based catalysts under comparable conditions. The crucial factors for such high methanol yield are the formation of small-sized PdZn alloy particles after H 2 reduction and abundant surface oxygen defects on ZnO. The SMSI between PdZn and ZnO also ensures a long term stability of our PdZn catalysts. At last, we propose the active site that was strongly associated with methanol formation is a PdZn alloy rather than metallic Pd.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Chuan Wang,Hongchao Li,Fanglin Shen,Shijian Ge,Xuan Zhang,Jun Ma,Kan Zhang,Jieshu Qian,Bingcai Pan
Proton-coupled electron transfer (PCET) is a key factor in determining the H 2 O 2 production efficiency from oxygen reduction reaction (ORR) or direct H 2 /O 2 reaction, which usually requires the aid of proton donors including alcohols. Here, we report a strong metal-support interaction (SMSI) strategy to facilitate the PCET process of a typical Pd/TiO 2 photocatalyst for photocatalytic ORR into H 2 O 2 production in pure water. Compared to conventional Pd/TiO 2 photocatalysts, the Pd/TiO 2 photocatalyst with SMSI between Pd and TiO 2 (Pd/TiO 2 -850H) promotes photocatalytic H 2 O 2 production in pure water by 4.21-fold, which can be ascribed to that the SMSI simultaneously promotes the H 2 O dissociation and the photogenerated charge transfer from TiO 2 to Pd catalyst, enabling highly efficient proton transfer to be participated into converting •O 2 - to H 2 O 2 . Moreover, the formation of TiO 2-x overlayer caused by SMSI suppresses the H 2 O 2 decomposition and stabilizes Pd NPs, finally achieving an H 2 O 2 production rate of 4.10 mmol g −1 h −1 , which surpasses most metal/TiO 2 photocatalytic system.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Nano Research
·
2021
·Vol. 14
·期 12
·4601-4609
·
IF 8.897
Fan Ruoyu,Zhang Yange,Hu Zhi,Chen Chun,Shi Tongfei,Zheng Lirong,Zhang Haimin,Zhu Junfa,Zhao Huijun,Wang Guozhong
To data, using strong metal-support interaction (SMSI) effect to improve the catalytic performance of metal catalysts is an important strategy for heterogeneous catalysis, and this effect is basically achieved by using reducible metal oxides. However, the formation of SMSI between metal and inert-support has been so little coverage and remains challenge. In this work, the SMSI effect can be effectively extended to the inert support-metal catalysis system to fabricate a Cu 0 /Cu-doped SiO 2 catalyst with high dispersion and loading (38.5 wt.%) through the interfacial effect of inert silica. In the catalyst, subnanometric composite of Cu cluster and atomic copper (in the configuration of Cu-O-Si) can be consciously formed on the silica interface, and verified by extended X-ray absorption fine structure (EXAFS), in situ X-ray photoelectron spectroscopy (XPS), and high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) characterization. The promoting activity in transfer-hydrogenation by the SMSI effect of Cu-silica interface and the synergistic active roles of cluster and atomic Cu have also been revealed from surface interface structure, catalytic activity, and density functional theory (DFT) theoretical calculation at an atomic level. The subnanometric composite of cluster and atomic copper species can be derived from a facile synthesis strategy of metal-inert support SMSI effect and the realistic active site of Cu-based catalyst can also been identified accurately, thus it will help to expand the application of subnanometric materials in industrial catalysis.
研究领域:
催化化学
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材料科学
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表面科学
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
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2023
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IF 15
Jianyu Han,Jingyi Yang,Zhixin Zhang,Xunzhu Jiang,Wei Liu,Botao Qiao,Junju Mu,Feng Wang
Multicomponent alloy (MA) contains a nearly infinite number of unprecedented active sites through entropy stabilization, which is a desired platform for exploring high-performance catalysts. However, MA catalysts are usually synthesized under severe conditions, which induce support structure collapse and further deteriorate the synergy between MA and support. We propose that a strong metal–support interaction (SMSI) could facilitate the formation of MA by establishing a tunnel of oxygen vacancy for metal atom transport under low reduction temperature (400–600 °C), which exemplifies the holistic design of MA catalysts without deactivating supports. PtPdCoFe MA is readily synthesized on anatase TiO2 with the help of SMSI, which exhibits good catalytic activity and stability for methane combustion. This strategy demonstrates excellent universality on various supports and multicomponent alloy compositions. Our work not only reports a holistic synthesis strategy for MA synthesis by synergizing unique properties of reducible oxides and the mixing entropy of alloy but also offers a new insight that SMSI plays a vigorous role in the formation of alloy NPs on reducible oxides.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Ziyang Chen,Jinjun Wen,Yu Zeng,Mengyuan Li,Yukun Tian,Fan Yang,Molly Meng-Jung Li,Peirong Chen,Haomin Huang,Daiqi Ye,Limin Chen
Cu/ZnO-based catalysts have been extensively and intensively studied for CO 2 hydrogenation to methanol due to their relatively superior catalytic performance. However, the mediocre methanol selectivity over Cu/ZnO-based catalysts has not been disclosed mainly because the predominant by-product CO formation activity fails to arouse any attention, significantly deterring the further catalyst optimization. The ZnOx-Cu nanoparticles (NP)-ZnO interface, derived from strong metal-support interactions (SMSI), has been recognized to be more active for methanol formation compared with the classical direct contact Cu-ZnO interface. In order to disclose the origin of the mediocre methanol selectivity, these two types of Cu-ZnO interfaces have been designed and constructed through carefully manipulating the synthesis and heat pre-treatment conditions of the powder model catalysts. Then, methanol and CO formation behaviors over these two interfaces have been explored thoroughly in actual reaction conditions. Finally, the origin of the mediocre methanol selectivity over Cu/ZnO-based catalysts has been proposed. This work provides unique insights for designing efficient Cu/ZnO-based catalysts with high methanol selectivity and yield and puts forward an effective strategy to investigate the catalytic behaviors over different interfaces in actual reaction conditions.
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
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Li Tian,Tao Hu,Yawen Guo,Peng Ju,Xiujuan Chen,Yueming Li,Xuedong Bai,Guorui Zhao
The design of self-supporting structure is particularly important to improve the stability and electrochemical performance of hydrogen evolution reaction electrode. Here, a facile strategy for building novel ultra-stable 0D-2D-3D integrated self-supporting electrode with high conductivity, sufficient diffusion channels and large reactive surface area was proposed. In the heterostructure, 2D Ti 3 C 2 T x flakes in-situ synthesized on 3D network porous Ti 3 AlC 2 surface which provides the multiple reactive surface areas and aggregation resistance to facilitating 0D ultrafine Pt nanoparticles uniform anchorage. Combined with structural characterization and first-principles calculations revealed that, the highly dispersed ultrafine Pt synergistically coupling strong metal-support interactions creates a unique multifunctional catalytic interface with high stability and atomic utilization efficiency of Pt to promote the HER in acidic and seawater. The resultant self-supporting electrode (support 0.48 wt% Pt) exhibits much superior activity to 10 % commercial Pt/C (loaded on foam nickel) in 0.5 M H 2 SO 4 (55 mV@10 mA cm −2 ) and simulate seawater (196 mV@10 mA cm −2 ) while reducing the Pt usage by 15 times. Meanwhile, the electrode also illustrates outstanding stability under high current densities (100 h@100 mA cm −2 ). This study provides a new design idea for developing integrated self-supporting catalytic electrodes to meet the durability of hydrogen evolution reaction applications in harsh environments.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Jingyi Yang,Yongzhen Gao,Jie Fan,Jieqiong Wang,Tao Yang,Zezheng Bing,Meng Zhang,Zhongyi Liu
Tuning the metal-support interaction (MSI) between highly dispersed nanosized metal particles and the support plays a pivotal role in the activity and selectivity of polyaromatics selective hydrogenation. In this work, the supported bimetallic Ni-Ru/SiO 2 -SEA catalyst was prepared by a strong electrostatic adsorption (SEA) strategy, and applied for the selective hydrogenation of biphenyl (BP) to cyclohexylbenzene (CHB). Compared to the catalysts prepared by the conventional incipient wetness impregnation method and Ni/SiO 2 -SEA, the significant effects of MSI and hydrogen spillover on Ni-Ru/SiO 2 -SEA facilitated the highly exposed and uniformly dispersed electron-deficient Ni δ+ (0 < δ < 2) species, which could enhance adsorption and activation of the electron-withdrawing phenyl group and H 2 , thereby promoting the efficient and selective conversion of BP to CHB. At the conditions of 160 ℃ and 2 MPa H 2 pressure, BP conversion over Ni-Ru/SiO 2 -SEA reached nearly 100 % within 3 h, achieving a remarkable selectivity of 97.9 % towards CHB, along with a high turnover frequency of 2756.9 h −1 for the active metallic Ni sites. Importantly, according to the kinetic simulations, the hydrogenation rate constant of Ni-Ru/SiO 2 -SEA was the highest (2.76 × 10 -2 mol·g −1 ·h −1 ) among the employed catalysts. Moreover, after six consecutive cycles, no obvious decline in hydrogenation efficiency was observed, confirming the remarkable activity and stability of Ni-Ru/SiO 2 -SEA. Furthermore, the activation of BP and desorption of CHB pathway on the Ni δ+ species were elaborated through temperature-programmed desorption characterization, highlighting the prominent contribution of MSI in enhancing the selective hydrogenation of polyaromatics.
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
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Lixin Zhang,Zhengxuan Zhu,Wei Tan,Jiawei Ji,Yandi Cai,Qing Tong,Yan Xiong,Haiqin Wan,Lin Dong
Strong metal–support interactions (SMSIs) have a significant effect on the performance of supported noble-metal catalysts for volatile organic compound (VOC) elimination. Herein, the strength of the SMSI of Pt/OMS-2 between Pt and the OMS-2 support is regulated by simply changing calcination temperatures, and the catalyst calcined at 300 °C (Pt/OMS-2-300) performs the best in the catalytic combustion of toluene. Through systematic structural characterizations, it is revealed that much more Pt2+–Ov–Mnδ+ species are formed in Pt/OMS-2-300, which can help facilitate the generation of more reactive oxygen species and promote lattice oxygen mobility. Moreover, the results of in situ DRIFTS experiments further confirm that abundant Pt2+–Ov–Mnδ+ species at the Pt–MnO2 interface on Pt/OMS-2-300 can better enhance the adsorption and activation of toluene, thus boosting the catalytic performance in toluene combustion. This newly developed strategy of thermal-driven regulation of the SMSI provides a novel perspective for constructing highly efficient catalysts for VOC emission control.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 18
·2633-2640
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IF 4.568
Guanghao Qiu,Qijun Pei,Yang Yu,Zijun Jing,Jintao Wang,Teng He,Ping Chen
Graphical A strategy for regulating strong metal-support interaction (SMSI) was proposed. The alkaline earth metal salts were doped into a Ru/TiO 2 catalyst, which successfully prevented the migration of TiO 2-x overlayer to Ru nanoparticles via in situ formation of titanates, while the electrons transfer from support to metal nanoparticles was strengthened. The alkaline earth metal salts-doped Ru/TiO 2 catalysts exhibited superior activity in the catalytic hydrogenation of aromatics. Classical strong metal-support interaction (SMSI) is of significant importance to heterogeneous catalysis, where electronic promotion and encapsulation of noble metal by reducible support are two main intrinsic properties of SMSI. However, the excessive encapsulation will inevitably hamper the contact between active sites and reactant, leading to reduced activity in catalysis. Herein, alkaline earth metal salts are employed to depress the encapsulation of Ru nanoparticles in Ru/TiO 2 catalyst in the present study. Thermodynamic calculation, transmission electron microscopy (TEM) and chemisorption results show that the alkaline earth metal salts could successfully prevent the migration of TiO 2-x overlayer to Ru nanoparticles in Ru/TiO 2 catalyst via in situ formation of titanates, resulting in high exposure of active metal. Meanwhile, X-ray photoelectron spectroscopy (XPS) and hydrogen temperature-programmed reduction (H 2 -TPR) results reveal that an even stronger electron donation from the reduced support to Ru nanoparticles is achieved. As a result, the alkaline earth metal salts-doped Ru/TiO 2 catalysts exhibit superior activity in catalytic hydrogenation of aromatics, which is in contrast to the pristine Ru/TiO 2 catalyst that shows negligible activity under the same conditions due to the excess encapsulation of Ru nanoparticles in Ru/TiO 2 catalyst.
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
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Tianyi Huang,Jiajia Wu,Yongqi Pan,Zhiyuan Yu,Fangyu Zhao,Shafqat Ullah,Yang Xu,Yong Chen,Zhehao Sun,Zongyou Yin,Qiangqiang Xue,Sibudjing Kawi,Shuliang Lu,Yujun Wang,Guangsheng Luo
The hydrogenation of the C=C bond in α-β unsaturated aldehydes faces substantial difficulties due to the steric hindrance and the conjugation effects of macromolecular unsaturated aldehydes. Herein, we introduce a novel approach to prepare nanosheet-structured Ni-Al 2 O 3 catalysts featuring exposed {100} crystal planes and hydroxyl groups, utilizing a microfluidic system to easily control crystal plane growth achieve support modification. In-situ characterizations and DFT calculations reveal that the exposed {100} crystal plane, a strong metal-support interaction (SMSI) promotes electron transfer of Ni and significantly reducing the C=C hydrogenation energy barrier from 3.12 eV to 1.79 eV. The hydroxyl environment facilitates effective adsorption of the C=O bond, accelerating the reaction and enabling rapid desorption of the product. Under modified reaction conditions for the preparation of 2-ethylhexanol, the catalyst still achieved a yield of 99.9%. This simple method of support modification enables rapid large-scale preparation, possessing significant potential for industrial applications.
研究领域:
催化化学
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材料科学
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理论计算化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）