Mechanistic Study of Carbon Dioxide Hydrogenation over Pd/ZnO‐Based Catalysts: The Role of Palladium–Zinc Alloy in Selective Methanol Synthesis

Zabilskiy, Maxim; Sushkevich, Vitaly L.; Newton, Mark A.; Krumeich, Frank; Nachtegaal, Maarten; Bokhoven, Jeroen A. van

doi:10.1002/ange.202103087

Cited by 10 publications

(3 citation statements)

References 36 publications

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“…In particular, for ZnZrO x , various metals such as Cu 23 , Pt 23 , Ga 24 , and Pd 22,23,25 have been reported as effective metal promoters. It is a general belief that the metal promoter and oxide support should be placed close to each other to maximize interfacial synergy (including strong metal-support interaction), and thus, various synthetic techniques were developed to anchor metal promotors directly on the oxide catalyst surface [26][27][28][29][30][31][32][33][34][35][36][37][38] . Previously, we studied Pd-promoted ZnZrO x catalyst (Pd/ZnZrO x ) for methanol formation 22 , revealing that the major role of Pd is to activate and split H 2 into H atoms that are subsequently transferred to adjacent Zn sites…”

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confidence: 99%

Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

et al. 2023

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Metal promotion is the most widely adopted strategy for enhancing the hydrogenation functionality of an oxide catalyst. Typically, metal nanoparticles or dopants are located directly on the catalyst surface to create interfacial synergy with active sites on the oxide, but the enhancement effect may be compromised by insufficient hydrogen delivery to these sites. Here, we introduce a strategy to promote a ZnZrOx methanol synthesis catalyst by incorporating hydrogen activation and delivery functions through optimized integration of ZnZrOx and Pd supported on carbon nanotube (Pd/CNT). The CNT in the Pd/CNT + ZnZrOx system delivers hydrogen activated on Pd to a broad area on the ZnZrOx surface, with an enhancement factor of 10 compared to the conventional Pd-promoted ZnZrOx catalyst, which only transfers hydrogen to Pd-adjacent sites. In CO2 hydrogenation to methanol, Pd/CNT + ZnZrOx exhibits drastically boosted activity—the highest among reported ZnZrOx-based catalysts—and excellent stability over 600 h on stream test, showing potential for practical implementation.

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Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

et al. 2023

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“…In addition, the interplanar spacing information of ZnO 1−x and Pd Cs can be seen from Figure 4c, respectively. The measured d spacing (0.260 nm) between the adjacent lattice planes is corresponded to the distance of ZnO (002) crystal planes [22][23][24]. Another d value of about 0.225 nm can be attributed to (111) planes of Pd Cs [25,26].…”

Section: Characterizations and Analysismentioning

confidence: 90%

Defective ZnO Nanoflowers Decorated by Ultra-Fine Pd Clusters for Low-Concentration CH4 Sensing: Controllable Preparation and Sensing Mechanism Analysis

et al. 2022

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To detect low concentration of CH4 is indeed meaningful in industrial manufacturing, such as the petrochemical industry and natural gas catalysis, but it is not easy to detect low concentration of CH4 due to its high symmetrical and stable structure. In this work, defect-rich ZnO1−x nanoflowers (NFs) were synthesized by a two-step route so as to obtain defect-enhanced gas-sensing performance, namely hydrothermal synthesis followed by H2 treatment. In order to achieve low-concentration detection of CH4, the ultra-thin Pd clusters’ (Cs, diameter about 1–2 nm) sensitizer was synthesized and decorated onto the surface of ZnO1−x NFs. It is found that Pd Cs-2/ZnO1−x gas sensors show enhanced gas-sensing properties to CH4, even at ppm concentration level. At its optimal working temperature of 260 °C, the gas response to 50 ppm CH4 can reach 5.0 with good gas selectivity; the response and recovery time is only 16.2 and 13.8 s, respectively. In the Results, we discussed the CH4 gas-sensing mechanism deeply. Overall, it is very necessary to detect low-concentration methane safely. It is possible for further safe detection of low-concentration methane gas in the future.

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“…), and oxide-(such as In x O y and Co 3 O 4 ) based catalysts. [7][8][9][10][11] As an effective and economic oxide, MnO x is widely used as a promoter with these catalysts in promoting CO 2 hydrogenation; however, it has rarely been employed directly as a catalyst. 12,13 Though MnO x as a promoter could enhance the activity and selectivity of the CO 2 hydrogenation reaction, its methanol synthesis and CO 2 conversion ability were found to be poor.…”

Section: Introductionmentioning

confidence: 99%

Boosting methanol productionviaplasma catalytic CO₂hydrogenation over a MnO_x/ZrO₂catalyst

Zhang

Sun

Shan

et al. 2023

Catal. Sci. Technol.

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Mechanistic Study of Carbon Dioxide Hydrogenation over Pd/ZnO‐Based Catalysts: The Role of Palladium–Zinc Alloy in Selective Methanol Synthesis

Abstract: Supporting information for this article is given via a link at the end of the document.

Cited by 10 publications

References 36 publications

Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

Defective ZnO Nanoflowers Decorated by Ultra-Fine Pd Clusters for Low-Concentration CH4 Sensing: Controllable Preparation and Sensing Mechanism Analysis

Boosting methanol productionviaplasma catalytic CO₂hydrogenation over a MnO_x/ZrO₂catalyst

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Mechanistic Study of Carbon Dioxide Hydrogenation over Pd/ZnO‐Based Catalysts: The Role of Palladium–Zinc Alloy in Selective Methanol Synthesis

Abstract: Supporting information for this article is given via a link at the end of the document.

Cited by 10 publications

References 36 publications

Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

Defective ZnO Nanoflowers Decorated by Ultra-Fine Pd Clusters for Low-Concentration CH4 Sensing: Controllable Preparation and Sensing Mechanism Analysis

Boosting methanol productionviaplasma catalytic CO2hydrogenation over a MnOx/ZrO2catalyst

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Boosting methanol productionviaplasma catalytic CO₂hydrogenation over a MnO_x/ZrO₂catalyst