Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 24
·5531-5538
·
IF 6.813
Hongliang Zhu,Roong Jien Wong,Xiangbowen Du,Leilei Du,Zhikang Jin,KaiCheng Qian,Junjie Song,Renhong Li,Wen Liu
Low-cost and highly active catalysts are attractive for catalysing formic acid (FA) dehydrogenation at room temperature. The PtNi alloy nanoparticles with the characteristic of lattice contraction and synergy effects were loaded on two-dimensional TiB2 by incipient-wetness impregnation. Compared to Pt/TiB2, the substitution of Ni reduces the amount of noble metal required, with the added advantage of significantly improving the catalyst activity by sixteen times. By investigating the various PtNi ratios, the Pt3Ni8/TiB2 (total metal loading = 2.0 wt%) catalyst was found to provide a low activation energy of 27.7 kJ mol−1 in 10.0 M FA aqueous solution at room temperature. This is the first example of using the alloy supported on TiB2 to achieve strong metal–support interaction (SMSI) to catalyse formic acid dehydrogenation at ambient temperature. XPS and TEM characterisation studies show that higher temperatures induced TiB2 to encapsulate the PtNi NPs, with the TiB2 surfaces serving as the active site for catalysing FA dehydrogenation. The catalytic activity of the obtained Pt3Ni8/TiB2 catalyst for the dehydrogenation of FA was much higher than those of its monometallic counterparts (Pt/TiB2 and Ni/TiB2) prepared by the same method, while demonstrating higher stability against agglomeration and CO poisoning. The excellent catalytic activity and stability of Pt3Ni8/TiB2 were mainly attributed to the presence of the SMSI effect of the catalyst. Additionally, the lattice distortion and local interactions within the ferromagnetic clusters of Pt3Ni8 alloy NPs created a synergistic effect, which resulted in an enhanced SMSI effect throughout the catalyst. This study introduces a new concept that magnetic Ni metal partially replacing noble metals can improve thermal stability and catalytic performance, while enabling facile catalyst recovery. Moreover, this research demonstrates that the controlled synthesis and rational design of 2D reticular crystal structure TiB2-supported alloy NPs may provide new opportunities to enhance the catalytic activity and improve the SMSI effect of noble metal-based nanostructures.
研究领域:
催化
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材料科学
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化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Weilin Tu,Mingyu Chu,Xianpeng Wang,Xuchun Wang,Yifan Li,Wenxiu Yang,Muhan Cao,Lu Wang,Youyong Li,Tsun-Kong Sham,Yi Cui,Qiao Zhang,Jinxing Chen
The in-depth mechanism of the emerging Ru-catalyzed polyolefin hydrogenolysis remains unclear. Here, we overcome this challenge by constructing a strong metal-support interaction (SMSI) system based on Ru/TiO 2 catalysts. With the increase of SMSI intensity, electrons are transferred from the TiO x capping layer to the Ru species. This effect facilitates the key steps of hydrogenation/desorption, while having little effect on the dehydrogenation and C–C cracking elementary reactions. As a result, the catalyst with higher hydrogenation capability prone to proceed hydrogenation and desorption step, thus suppressing cascade C–C cracking and avoiding the production of low value methane. The catalyst with the strongest SMSI effect exhibits a liquid fuel yield of 89.4% at ∼100% solid conversion. The SMSI effect also enables the catalysts with superior stability, so it can also efficiently upcycle commercial polyolefins. This work provides an in-depth understanding of the effects of metal-support interactions on polyolefin hydrogenolysis and paves the way for catalyst design.
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
Nature Catalysis
·
2021
·Vol. 4
·期 5
·418-424
·
IF 41.813
Wang Hai,Wang Liang,Lin Dong,Feng Xiang,Niu Yiming,Zhang Bingsen,Xiao Feng-Shou
Strong metal–support interactions (SMSIs) are crucial for the preparation of supported metal catalysts. A prevailing view is that the redox feature of the metal oxide support is the driving force behind SMSI construction. Herein we demonstrate CO 2 -induced SMSIs between irreducible oxide MgO and noble gold nanoparticles, presenting electronic and geometric features that are similar to those of classical SMSIs. The key to these interactions is activating the oxide surface by a reversible reaction, MgO + CO 2 ⇆ MgCO 3 , which leads to migration of the support onto the gold nanoparticles to form thin overlayers. The overlayer is permeable to the reactant molecules, stable under the oxidation conditions and even water tolerant, resulting in sinter-resistant gold nanoparticle catalysts. This investigation provides an approach for the rational design and optimization of supported metal catalysts based on irreducible oxides, and deepens our understanding of the mechanism of SMSI formation.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
NANO
·
2026
·
IF 1.3
Runcai Xu,Jiqing Dong,Xintao Gao,Xin Cheng,Xiangyan Chen,Yantao Li
Developing highly sensitive and stable nonenzymatic glucose sensors remains crucial for reliable glucose monitoring. Herein, we report an SMSI-driven Au/CeO 2 -BTC nanozyme derived from a Ce-BTC metal-organic frameworks (MOFs) for efficient electrochemical glucose detection. The Ce-trimesic acid (Ce-BTC) precursor was calcined to generate a porous CeO 2 -BTC framework with abundant oxygen vacancies, followed by the in situ deposition of Au nanoparticles. Structural analyses reveal the formation of Au-O-Ce interfacial sites, indicating pronounced trong metal-support interactions (SMSI) that induce electronic modulation, increase Ce 3+ concentration, and facilitate rapid charge transfer. Benefiting from these synergistic effects, the Au/CeO 2 -BTC-modified electrode exhibits excellent catalytic activity toward glucose oxidation, achieving a sensitivity of 41.3 µA cm -2 mM -1 and a detection limit of 4.75 µM, along with good reproducibility, stability, and selectivity. This work highlights the importance of SMSI engineering in MOF-derived nanozymes and provides an effective strategy for constructing high-performance electrochemical glucose sensors
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Kehui Xue,Lianqing Yu
Strong Metal-Support Interactions (SMSI) are recognized as a crucial aspect of tuning catalytic activity. Here we report the remarkable effectiveness of SMSI between Mn:BiVO 4 supports and semi-embedded Pt nanoparticles (NPs) (Pt/Mn:BiVO 4 -SMSI) in enhancing photoelectrochemical (PEC) water splitting. The incorporation of Mn greatly reduces the polaron jumping barriers and passivates the surface trap states. Due to the SMSI, electrons are transferred from the V 4+ to the Pt NPs, resulting in the construction of electron-rich Pt species (Pt δ– ) and semi-embedded interfaces (Pt δ– –O V –VO x ), which contributes to the extraction of photoinduced holes and shorten the charge transport distances. Benefiting from the SMSI effect, the as-obtained Pt/Mn:BiVO 4 -SMSI composite photoelectrode shows an excellent photocurrent density of 4.47 mA‧cm −2 at 1.23 versus the reversible hydrogen electrode in conventional electrolytes. Importantly, for PEC seawater splitting, VO x Lewis acid protective layer can tune the surface micro-catalytic environment. It enables the capture of OH − ions and resists surface Cl − to inhibit the chlorine attack on the photoelectrode. Such an in-situ generated microenvironment avoids the formation of precipitates. As a result, the Pt/Mn:BiVO 4 -SMSI exhibits an superior stability in both simulated seawater and natural seawater, respectively. This work sheds new light on the design of efficient photoanodes for PEC seawater splitting.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Bin Wang,Shu-han Lu,Shi-yuan Wang,Pei-ya Li,Tao Fang
N -ethylcarbazole (NEC) is a widely studied liquid organic hydrogen carrier, and a large number of catalysts with excellent reactivity has been designed and developed thus far. However, the phenomenon of isomeric transformation of 12H-NEC products during the reaction was not explained. Here, we studied the process based on three different Ru catalysts supported on zirconium-based supports, and based on the experimental results, we identified that supported metal-support strong interaction (SMSI), metal-support anion interaction (MSAI) and hydrogen spillover will have coupling effect on the hydrogenation reaction path and the occurrence of isomerization in 12H-NEC product. Higher 12 [H] B content in 12H-NEC under Ru/ZrN catalyst was caused by the large number of secondary active centers on the surface of the support reacting in the hydrogenation reaction. The active site for the isomerization of 12 [H] B to 12 [H] A may be the electronegativity interface formed by Ru and the support, while the electroneutral or electropositive interface rich in hydrogen is not conducive to the catalytic conversion. To sum up, an image model for the isomeric transformation of 12H-NEC products was proposed.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Ziyang Xu,Shengpeng Mo,Yanxia Li,Yuchen Zhang,Junliang Wu,Mingli Fu,Xiaojun Niu,Yun Hu,Daiqi Ye
The problem of deep oxidation of low concentrations of VOCs in industrial tail gas is exceptionally urgent. The preparation of VOCs ozonation catalyst with a high mineralization rate is still a challenge. In this paper, manganese oxide carriers with different morphologies were synthesized by simple methods and used to catalyze ozone mineralization of toluene after loading Pt nanoparticles efficiently. The conversion of toluene over Pt/MnO x -T catalyst was more than 98 % at ambient temperature, and the mineralization rate of toluene was close to 100 % at 70 °C. Through a variety of characterization methods, the strong metal-support interaction (SMSI) between Pt nanoparticles and carriers was successfully constructed. It was found that SMSI successfully optimized the surface oxygen species and oxygen migration ability of the catalyst, and then realized the high degree of mineralization of toluene at low temperature. This paper guides the subsequent development of Pt–Mn catalysts for catalytic organic pollutants ozonation with high activity.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shaodi Sun,Xiaomin Wu,Zhiwei Huang,Huazheng Shen,Huawang Zhao,Guohua Jing
The strong metal-support interaction (SMSI) has received wide attention in heterogeneous catalysis for the room-temperature oxidation of formaldehyde. An interaction between Pt nanoclusters and oxygen vacancy defects will lead to SMSI over the Pt-based catalysts. In this study, defective two-dimensional (2D) TiO 2 nanosheets were synthesized and successfully anchored Pt nanoclusters with a size of 1.3 nm (0.1Pt/TiO 2 -NS). The 0.1Pt/TiO 2 -NS catalyst displayed a superior activity of > 95% HCHO conversion at room temperature, which was ∼ 50% higher than that obtained for a counterpart having the commercial TiO 2 (Degussa P25) support. The abundant oxygen vacancies and stable Pt nanoclusters on 0.1Pt/TiO 2 -NS by introducing SMSI boosted the excellent activity and stability of HCHO oxidation. By exploring electron transfer, suppression of small-molecule adsorption and encapsulation, SMSI was well demonstrated. Furthermore, electron transfer from Pt to TiO 2 -NS led to the electron-deficient Pt surface. The electron-deficient Pt caused by SMSI will enhance the adsorptions of HCHO and H 2 O/O 2 , subsequently improving the catalytic performance. SMSI between Pt nanoclusters and oxygen vacancies endowed the 0.1Pt/TiO 2 -NS catalyst excellent activity and stability to HCHO elimination. In addition, the mechanism for the high HCHO oxidation performance were examined through analysis of in situ HCHO-diffuse reflectance infrared Fourier transform spectra (DRIFTS).
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
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
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zequn Zhang,Yuan Shu,Qian Liu,Shuxian Bi,Pengfei Zhang
Colloidal nanoparticles with uniform particle size distribution, tailored exposed facets, and controllable compositions appealed to broad interests in heterogeneous catalysis. Nevertheless, due to the strong attachment of capping agents to the nanoparticles, cleaning the nanoparticle surface without changing the size of nanoparticles remains a significant challenge. Herein, based on the double confinement of the strong metal-support interaction (SMSI) effect and carbon encapsulation, the well-stabilized Ni-ZnO-S3 catalyst was successfully synthesized. The size of Ni nanoparticles after calcination in the sequence of H 2 -N 2 mixture, air, and H 2 -N 2 mixture remained below 5 nm. Due to no significant size change in Ni nanoparticles, the prepared Ni-ZnO-S3 catalyst served well as model catalysts in the RWGS reaction, where the CO 2 conversion and CO yield increased proportionally to the Ni loading weight. According to the result of in-situ FTIR, an associative mechanism of RWGS reaction over Ni-ZnO-S3 was also identified. Therefore, this dual protect strategy provides a potential solution for building highly anti-sintering catalysts based on the colloidal synthesis route.
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
Molecular Catalysis
·
2023
·
IF 4.6
Hua Yang,Zemin An,Yuanjie Xu,Lizhi Wu,Li Tan,Yu Tang
The restructuring of a catalyst under working conditions has been recognized as a critical factor that can significantly impact their performance in recent years. In this study, we investigate the behavior of a highly dispersed Ni supported on TiO 2 (P25) catalyst during the partial oxidation of methane (POM) to produce syngas. Our results reveal a distinct oscillation phenomenon in the catalyst's performance over time. The simultaneous oscillations of rapid deactivation and activation are observed, while the catalyst remains active for continuous POM reaction. Comprehensive characterizations suggest that this deactivation is not caused by traditional deactivation mechanisms with coke formation or Ni sintering. The formation of inactive NiTiO 3 results in catalyst deactivation, which is formed between Ni and TiO 2 support in the reductive atmosphere of POM products under high temperature due to strong metal-support interaction (SMSI). The simultaneous presence of oxidative and reductive atmospheres of the reactants and products in the POM reaction leads to the generation or demise of NiTiO 3 . The dynamic change of the Ni active sites during the in-situ reaction leads to the oscillation of the catalytic activity. This study sheds new light on the importance of SMSI in understanding the behavior of catalysts under working conditions.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 9
·2104972
·
IF 17.521
Shenghua Wang,Kai Feng,Dake Zhang,Deren Yang,Mengqi Xiao,Chengcheng Zhang,Le He,Binhang Yan,Geoffrey A. Ozin,Wei Sun
Cu-based catalysts exhibit excellent performance in hydrogenation reactions. However, the poor stability of Cu catalysts under high temperatures has restricted their practical applications. The preparation of stable Cu catalysts supported by SiO 2 with strong metal–support interaction (SMSI) has thus aroused great interest due to the high abundance, low toxicity, feasible processability, and low cost of SiO 2 . The challenge in the construction of such SMSI remains to be the inertness of SiO 2 . Herein, a simple and scalable method is developed to prepare 2D silica (2DSiO 2 ) supported Cu catalysts with SMSI by carefully manipulating the topological exfoliation of CaSi 2 with CuCl 2 and thereafter calcination. The prepared Cu-2DSiO 2 catalysts with the unique encapsulated Cu nanoparticles exhibit excellent activity and long-term stability in high-temperature CO 2 hydrogenation reactions. This feasible and low-cost solution for stabilizing Cu catalysts might shed light on their realistic applications.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）