Sinter-resistant Rh nanoparticles supported on γ-Al<sub>2</sub>O<sub>3</sub>nanosheets as an efficient catalyst for dry reforming of methane

Chu, Shasha; Cai, Zhengmiao; Zheng, Yanping; Wang, Yongke; Zhou, Zhao‐Hui; Weng, Weizheng

doi:10.1039/d0nr04644b

Cited by 30 publications

(9 citation statements)

References 49 publications

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“…The size distributions show that the average sizes of Rh nanoparticles for Rh/MgAl 2 O 4 -MC (Figure B) and Rh/MgAl 2 O 4 -NP (Figure S4B) are 1.11 and 1.63 nm, respectively (Table ). Based on the average size ( d ) of Rh nanoparticles, the dispersions ( D ) of Rh nanoparticles are calculated according to the equation ( d = 1.09/ D ). , The dispersions of Rh nanoparticles for Rh/MgAl 2 O 4 -MC and Rh/MgAl 2 O 4 -NP are 98.2 and 66.9%, respectively (Table ). The dispersion of Rh nanoparticles was further measured by H 2 chemisorption (see the Experimental Section).…”

Section: Resultsmentioning

confidence: 99%

“…As shown in Figure C, Rh/MgAl 2 O 4 -NP shows high r CH4 and r CO2 (10.9 and 13.2 mol mol Rh –1 s –1 ), which are comparable to the highest rates reported for Rh-based catalysts (Table S1). − Its TOF CH4 and TOF CO2 are 15.6 and 18.8 s –1 , respectively. Remarkably, Rh/MgAl 2 O 4 -MC shows extremely high r CH4 and r CO2 of 51.1 and 62.7 mol mol Rh –1 s –1 , which are 4.7 and 4.8 times higher than those of Rh/MgAl 2 O 4 -NP, respectively.…”

Section: Resultsmentioning

confidence: 99%

“…Among them, inexpensive nonprecious metal catalysts (e.g., Ni and Co) show good catalytic activity, but they are prone to deactivation due to the thermodynamically inevitable side reactions of carbon deposition such as CH 4 complete dissociation and CO disproportionation. Persistent efforts have been devoted to improving catalytic durability. − Supported precious metal catalysts (e.g., Rh, Ru, Pt, and Pd) show not only good catalytic activity but also excellent carbon-resistant properties. − ,− However, the earth-scarcity and expensiveness of precious metals greatly limit their practical application in DRM. One strategy to overcome the obstacle is to considerably reduce the loading of precious metals, thus significantly decreasing the catalyst cost.…”

Section: Introductionmentioning

confidence: 99%

“…One strategy to overcome the obstacle is to considerably reduce the loading of precious metals, thus significantly decreasing the catalyst cost. By the strategy, the specific reaction rate increases due to the dispersion of precious metal nanoparticles. ,, However, it usually leads to a considerable reduction in total catalytic activity (e.g., CH 4 and CO 2 conversions). Another strategy is to design single-atom precious metal catalysts to realize high precious metal atom utilization, which has been a hot topic in the field of heterogeneous catalysis including DRM. ,,− …”

Section: Introductionmentioning

confidence: 99%

“…33,61 The dispersions of Rh nanoparticles for Rh/MgAl 2 O 4 -MC and Rh/MgAl 2 O 4 -NP are 98.2 and 66.9%, respectively (…”

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confidence: 99%

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Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl₂O₄ Nanosheets for Catalytic CO₂ Reforming of Methane

Zhang

et al. 2021

ACS Appl. Nano Mater.

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A unique nanocomposite of Rh quasi-monolayer clusters supported on spinel MgAl2O4 nanosheets with a low Rh loading of 0.15 wt % (Rh/MgAl2O4-MC) was synthesized by a facile method. By the catalyst design, nearly all of Rh atoms are utilized like well-known surface single-atom catalysts. More importantly and surprisingly, Rh/MgAl2O4-MC shows extremely high specific reaction rates of CH4 (r CH4) and CO2 (r CO2) per mole Rh and turnover frequency (TOF) for catalytic CO2 reforming of CH4 (DRM). Its r CH4 and r CO2 are as high as 51.14 and 62.65 mol molRh –1 s–1, which are 4.7 and 4.8 times higher than those of conventional Rh nanoparticles supported on spinel MgAl2O4 nanosheets with a higher Rh loading of 0.96 wt % (Rh/MgAl2O4-NP), respectively. Its TOF values of CH4 and CO2 are as much as 53.9 and 66.1 s–1, which are 3.5 and 3.5 times higher than those of Rh/MgAl2O4-NP, respectively. Meanwhile, Rh/MgAl2O4-MC retains the excellent catalytic durability of supported nanoparticles with negligible side reaction of carbon deposition, which is in striking contrast to the prone deactivation of the single-atom catalysts of precious metals (e.g., Rh and Ru) reported. Experimental evidence and DFT calculations reveal the presence of a strong interaction between Rh quasi-monolayer clusters and MgAl2O4 for Rh/MgAl2O4-MC. The interaction not only makes energetically unstable clusters stable but also alters the reaction pathway of DRM. Compared to DRM on Rh nanoparticles, the oxidations of C* and CH* species as the rate-determining step of DRM are significantly accelerated on Rh quasi-monolayer clusters due to their activation energies being considerably reduced, thus improving intrinsic catalytic activity and inhibiting the side reaction of carbon deposition.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

“…33,61 The dispersions of Rh nanoparticles for Rh/MgAl 2 O 4 -MC and Rh/MgAl 2 O 4 -NP are 98.2 and 66.9%, respectively (…”

mentioning

confidence: 99%

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Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl₂O₄ Nanosheets for Catalytic CO₂ Reforming of Methane

Zhang

et al. 2021

ACS Appl. Nano Mater.

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Dry Reforming of Methane on Low‐Loading Rh Catalysts

Tsuchida,

Kurokawa,

Yamamoto

et al. 2024

ChemCatChem

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Dry reforming of methane (DRM) is a promising catalytic process for converting greenhouse gases (CH4 and CO2) into syngas (CO and H2). This study investigates DRM under moderate conditions (550 °C) using supported ultra‐low loading (0.05 wt%) metal (M) catalysts (M = Rh, Ru, Pt, Pd, Ir, Au, and Ni). The reaction was carried out for 6 h with a flow rate of 30 mL/min for both CH4 and CO2, using 0.10 g of catalyst. Among these catalysts, 0.05 wt% Rh/Al2O3 exhibited the highest DRM activity. The effect of catalyst supports revealed that Al2O3 is the most effective support for 0.05 wt% Rh. The DRM activity of Rh species supported on Al2O3 and SiO2 was compared, and the Rh species on Al2O3 outperformed those on SiO2, indicating Al2O3 enhances the DRM activity of Rh. When comparing the DRM activity of Rh nanoparticles and Rh single atoms, it was suggested that Rh nanoparticles might exhibit superior performance for DRM. Coke deposited on 0.05 wt% Rh/Al2O3 is removed by CO2, maintaining stable catalytic activity. These findings provide valuable insights into the design of catalysts that minimize the use of noble metals in DRM reactions.

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Nickel Supported on Multilayer Vanadium Carbide for Dry Reforming of Methane

Huang

Qin

et al. 2022

ChemistrySelect

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A multilayer vanadium carbide MXene (m-V 2 C) was used as a robust oxy-carbide support to prepare a series of Ni/m-V 2 O 3 -V 2 C catalysts with various Ni amounts by an impregnation method and used for dry reforming of methane (DRM). The results show that the Ni addition increases the catalyst alkalinity, and the interaction between the Ni metal and m-V 2 C increases with increasing Ni amount. Ni/m-V 2 O 3 -V 2 C with a Ni amount of 13 wt% showed optimal CH 4 and CO 2 conversions of 94 % and 89 %, respectively. In addition, 13Ni/m-V 2 O 3 -V 2 C exhibits excellent catalytic stability and anti-coking ability in a 90-hour stability test, which is attributed to the strong metalsupport interaction. In situ DRIFTS analysis showed that methane activated on the Ni particles generates CH x and H, while CO 2 interacts with m-V 2 O 3 -V 2 C to form carbonates on Ni/ m-V 2 O 3 -V 2 C; carbonate species come into contact with methane pyrolysis products and quickly form formate species, which are further decomposed into CO.

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Sinter-resistant Rh nanoparticles supported on γ-Al₂O₃nanosheets as an efficient catalyst for dry reforming of methane

Abstract: γ-Al2O3 nanosheets supported rhodium catalysts with Rh loadings between 0.05 and 2 wt% were prepared by impregnation method and used for dry reforming of methane (DRM). It was found that...

Cited by 30 publications

References 49 publications

Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl₂O₄ Nanosheets for Catalytic CO₂ Reforming of Methane

Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl₂O₄ Nanosheets for Catalytic CO₂ Reforming of Methane

Dry Reforming of Methane on Low‐Loading Rh Catalysts

Nickel Supported on Multilayer Vanadium Carbide for Dry Reforming of Methane

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Sinter-resistant Rh nanoparticles supported on γ-Al2O3nanosheets as an efficient catalyst for dry reforming of methane

Abstract: γ-Al2O3 nanosheets supported rhodium catalysts with Rh loadings between 0.05 and 2 wt% were prepared by impregnation method and used for dry reforming of methane (DRM). It was found that...

Cited by 30 publications

References 49 publications

Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl2O4 Nanosheets for Catalytic CO2 Reforming of Methane

Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl2O4 Nanosheets for Catalytic CO2 Reforming of Methane

Dry Reforming of Methane on Low‐Loading Rh Catalysts

Nickel Supported on Multilayer Vanadium Carbide for Dry Reforming of Methane

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Sinter-resistant Rh nanoparticles supported on γ-Al₂O₃nanosheets as an efficient catalyst for dry reforming of methane

Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl₂O₄ Nanosheets for Catalytic CO₂ Reforming of Methane

Quasi-Monolayer Rh Nanoclusters Stabilized on Spinel MgAl₂O₄ Nanosheets for Catalytic CO₂ Reforming of Methane