Incorporating Sulfur Atoms into Palladium Catalysts by Reactive Metal–Support Interaction for Selective Hydrogenation

Wu, Zhenyu; Nan, Hang; Shen, Shan‐Cheng; Chen, Ming‐Xi; Liang, Haojun; Huang, Chuanqi; Yao, Takeshi; Chu, Shengqi; Li, Wei-Xue; Yu, Shu‐Hong

doi:10.31635/ccschem.021.202101428

Cited by 11 publications

(7 citation statements)

References 60 publications

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“…Upon further increasing the temperature, alloying between the oxide overlayer and the metal might take place . This process was described as reactive MSIs (RMSIs), attracting broad interest in a number of catalytic reactions. − …”

Section: Introductionmentioning

confidence: 99%

Atomically Thick Oxide Overcoating Stimulates Low-Temperature Reactive Metal–Support Interactions for Enhanced Catalysis

Liu

Zhang

et al. 2023

J. Am. Chem. Soc.

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Reactive metal−support interactions (RMSIs) induce the formation of bimetallic alloys and offer an effective way to tune the electronic and geometric properties of metal sites for advanced catalysis. However, RMSIs often require high-temperature reductions (>500 °C), which significantly limits the tuning of bimetallic compositional varieties. Here, we report that an atomically thick Ga 2 O 3 coating of Pd nanoparticles enables the initiation of RMSIs at a much lower temperature of ∼250 °C. State-of-the-art microscopic and in situ spectroscopic studies disclose that low-temperature RMSIs initiate the formation of rarely reported Ga-rich PdGa alloy phases, distinct from the Pd 2 Ga phase formed in traditional Pd/Ga 2 O 3 catalysts after hightemperature reduction. In the CO 2 hydrogenation reaction, the Ga-rich alloy phases impressively boost the formation of methanol and dimethyl ether ∼5 times higher than that of Pd/Ga 2 O 3 . In situ infrared spectroscopy reveals that the Ga-rich phases greatly favor formate formation as well as its subsequent hydrogenation, thus leading to high productivity.

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Section: Introductionmentioning

confidence: 99%

Atomically Thick Oxide Overcoating Stimulates Low-Temperature Reactive Metal–Support Interactions for Enhanced Catalysis

Liu

Zhang

et al. 2023

J. Am. Chem. Soc.

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“…Compared to classical SMSI, the RMSI phenomenon is rarer in carbon materials because the light elements on the surface of carbon vaporize at high temperatures and do not enter the metal to form metal–light element compounds, so RMSI phenomena cannot be observed. It was not until 2020 that RMSI in carbon materials applied to hydrogenation reactions was reported where the researchers found that during the pyrolysis process the S element in the support was embedded into the lattice of Pd, and Pd 4 S intermetallic compounds were formed by simply loading Pd onto the S–C support . As shown in Figure c, the Pd source was anchored onto a preprepared S–C support using the initial wet impregnation method.…”

Section: Characterization Of the Multi Heteroatom Coordination Enviro...mentioning

confidence: 99%

“…It was not until 2020 that RMSI in carbon materials applied to hydrogenation reactions was reported where the researchers found that during the pyrolysis process the S element in the support was embedded into the lattice of Pd, and Pd 4 S intermetallic compounds were formed by simply loading Pd onto the S−C support. 73 As shown in Figure 2c, the Pd source was anchored onto a preprepared S−C support using the initial wet impregnation method. At low temperature, it was found that only one single peak (1.8 Å) corresponding to the Pd−S bond was found in k 2 -weighted FT-EXAFS.…”

Section: Thementioning

confidence: 99%

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Tailoring the Nonmetal Elements in Carbon-Based Single-Atom Catalysts toward Hydrogen Energy Catalysis

Tang,

Yang,

Wang

et al. 2024

J. Phys. Chem. C

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Single-atom catalysts (SACs) have been intensively studied due to their merits including extremely high atom utilization, excellent catalytic activity, and unique selectivity. The catalytic activity of SACs is mainly regulated by factors including central metal atoms, the chelation atoms, and thereby the electronic structure of the SACs. Studies have shown that the alternation in heteroatom configuration can significantly tailor the catalytic performance, as the electronic structure of the center metal is highly sensitive to its chelating elements and coordination structure. In this review, we mainly focus on the influence of P and S doping on the catalytic activity of SACs from the perspectives of hydrogen energy conversion. The doping methods of S/P heteroatoms are first introduced in detail, with the active centers for multiheteroatom coordination identified using advanced characterization techniques. Then, through specific applications of SACs in oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), the superiority of multidoping over single doping is demonstrated, and the mechanism of S/P doping toward catalytic activity promotion is explained. Finally, future developments and challenges of multidoped atom coordination are discussed.

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“…An interesting RMSI was found recently in SÀ C supported Pd catalysts, in which the sulfur atoms doped in the carbon supports were extracted out and reacted with Pd [37] to form crystalline Pd 4 S nanoparticle catalysts (Figure 4a). [48] The temperature-dependent structural evolution process of the SÀ C supported Pt catalyst was elucidated with the help of spectroscopic and electron microscopy characterizations. At the low temperature of 300 °C, the Pd species began to react with S atoms that were extracted out from SÀ C supports to form loosely assembled Pd x S nanoclusters with exclusive PdÀ S x configuration.…”

Section: Reactive Metal-support Interactionmentioning

confidence: 99%

Strong Metal‐Support Interactions through Sulfur‐Anchoring of Metal Catalysts on Carbon Supports

2023

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In supported metal catalysts, the supports would strongly interact with the metal components instead of just acting as a carrier, which greatly affects both of their synthesis and catalytic activity, selectivity, and stability. Carbon is considered as very important but inert support and thus hard to induce strong metal-support interaction (SMSI). This mini-review highlights that sulfur-a documented poison reagent for metal catalysts-when doped in a carbon supports can induce diverse SMSI phenomenon, including electronic metal-support interaction (EMSI), classic SMSI, and reactive metal-support interaction (RMSI). These SMSI between metal and sulfur-doped carbon (SÀ C) supports enables the catalysts with extraordinary resistance to sintering at high temperatures of up to 1100 °C, which allows the general synthesis of single-atom, alloy cluster, and intermetallic compound catalysts with high dispersion and metal loading for a variety of applications.

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Incorporating Sulfur Atoms into Palladium Catalysts by Reactive Metal–Support Interaction for Selective Hydrogenation

Cited by 11 publications

References 60 publications

Atomically Thick Oxide Overcoating Stimulates Low-Temperature Reactive Metal–Support Interactions for Enhanced Catalysis

Atomically Thick Oxide Overcoating Stimulates Low-Temperature Reactive Metal–Support Interactions for Enhanced Catalysis

Tailoring the Nonmetal Elements in Carbon-Based Single-Atom Catalysts toward Hydrogen Energy Catalysis

Strong Metal‐Support Interactions through Sulfur‐Anchoring of Metal Catalysts on Carbon Supports

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