In-situ deposition and subsequent growth of Pd on SnO2 as catalysts for formate oxidation with excellent Pd utilization and anti-poisoning performance

Wang, Mengxue; Lian, Tingting; Wang, Jianshe; Cheng, Xianglin; Zhao, Jianhong; Song, Cheng-Ying; Wang, Liucheng; Xi, Jingyu

doi:10.1016/j.ijhydene.2019.06.057

Cited by 12 publications

(2 citation statements)

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“…Alternatively, the introduction of metal cocatalysts or metal oxide substrates with oxophilic nature, as an effective approach, has been recently reported to enhance the performance of catalysts. Specifically, the in situ generated reactive oxygen species (ROS) by metal cocatalysts or metal oxide substrates can assist the removal of H* or CO ad from the surface of catalysts. − Such a strategy has been adopted in designing catalysts for the hydrogen evolution reaction and the small organic molecule oxidation reaction. − For instance, to improve the activity and stability toward the ethanol oxidation reaction (EOR), Chen et al introduced Ni as an oxophilic component into the Pd–Ni–P catalyst. They found that the produced ROS of OH* can eliminate the carbonaceous poison .…”

Section: Introductionmentioning

confidence: 99%

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO₂ Substrate

Zhao

Zhang

et al. 2021

ACS Appl. Mater. Interfaces

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Direct formate fuel cells (DFFCs) as promising energy technologies have been applied for portable and wearable devices. However, for the formate oxidation reaction (FOR), the deficiency of catalysts has prevented DFFCs from practical applications. Herein, we prepared a Pd-loaded CeO2 catalyst through a simple steam treatment at 400 °C to enhance the catalytic FOR performance. In comparison with the counterpart of Pd/CeO2 without stream treatment, the as-prepared Pd/CeO2-ST catalyst has a lower onset potential of 381 mV and a lower peak potential of 0.64 V with a higher peak current of 10.62 mA cm–2. The experimental results show that the enhanced FOR properties of Pd/CeO2-ST are ascribed to the introduction of surface reactive oxygen species to the CeO2 substrate, which substantially promotes the desorption of adsorbed hydrogen (H*) intermediates. Density functional theory (DFT) calculations reveal that on the surface of CeO2, the abundant oxygen vacancies boost the OH* adsorption ability and accelerate the kinetics of the potential-limiting step. This work not only proposes a new strategy for enhancing the activity of FOR catalysts but also highlights the understanding of the FOR mechanism in alkaline media for DFFC applications.

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Section: Introductionmentioning

confidence: 99%

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO₂ Substrate

Zhao

Zhang

et al. 2021

ACS Appl. Mater. Interfaces

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“…On varying the Pd/Sn ratio, the affinity to H increases, with Pd 50 Sn 50 having a BE value of −3.01 eV in line with the experimental observation of deteriorated catalytic efficiency. We then further analyzed the binding energy of possible poisoning intermediates in the pathway of formate oxidation, CO ads over the Pd 100 and Pd 90 Sn 10 alloy surfaces as the alloy catalysts showed a better residual current density during chronoamperometry, i – t (Figure e) . Interestingly, less favorable adsorption (CO ads ) was observed for the alloy with a value of −0.04 eV compared to −1.76 eV for Pd 100 , indicating an active conversion of CO. Alloying with Sn for Pd and the subsequent changes including the downshift of the d- band center and electronic effects have enhanced the HCOO oxidation performance by weakening the adsorption of intermediates (H ads and CO ads ) over Pd surface, which was experimentally observed as lower onset potentials and higher residual (CA) stability during FOR.…”

Section: Resultsmentioning

confidence: 99%

Alkaline Formate Oxidation with Colloidal Palladium–Tin Alloy Nanocrystals

Sankar

Aravindh

Jose

et al. 2021

ACS Appl. Energy Mater.

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The design of advanced catalysts for newer-generation fuel cells such as direct formate fuel cells (DFFCs) is an important milestone for energy generation and environmental sustainability. Formate as an alternative for alcohols in direct liquid fuel cells is gaining momentum since they can be regenerated from CO 2 , providing dual benefits of energy generation and carbon footprint reduction under the framework of the circular economy. Anticipating advantages from the oxyphilicity and lower electronegativity in tin (Sn)-alloyed palladium (Pd) crystals than to pure palladium catalysts (Pd/C), we developed effective nano-PdSn alloy crystals over carbon support (Pd x Sn y /C) through a colloidal crystal growth scheme. The alloyed nanocrystals were characterized for the alkaline formate oxidation reaction (FOR) intended for their suitability as DFFC anode catalysts, and several-fold enhancement was observed with higher current density, lower onset potential, and enhanced stability compared to Pd/ C. Density functional theory (DFT) calculations provided proper insights into the promotional effects upon appropriate alloying of Sn with Pd, with structural changes and the consequent modifications of the density of states, enhanced OH ads in alkaline conditions, reduced intermediate poisoning (H ads and CO ads ), and lowering of work function being identified as factors leading to excellent formate oxidation kinetics. The results obtained and detailed here could be used to design and process Pd nanocatalysts for better-performing DFFCs.

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Ultrasensitive methyl salicylate gas sensing determined by Pd-doped SnO2

Zhu

Wang

et al. 2022

Front. Mater. Sci.

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In-situ deposition and subsequent growth of Pd on SnO2 as catalysts for formate oxidation with excellent Pd utilization and anti-poisoning performance

Cited by 12 publications

References 50 publications

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO₂ Substrate

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO₂ Substrate

Alkaline Formate Oxidation with Colloidal Palladium–Tin Alloy Nanocrystals

Ultrasensitive methyl salicylate gas sensing determined by Pd-doped SnO2

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In-situ deposition and subsequent growth of Pd on SnO2 as catalysts for formate oxidation with excellent Pd utilization and anti-poisoning performance

Cited by 12 publications

References 50 publications

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO2 Substrate

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO2 Substrate

Alkaline Formate Oxidation with Colloidal Palladium–Tin Alloy Nanocrystals

Ultrasensitive methyl salicylate gas sensing determined by Pd-doped SnO2

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Product

Resources

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Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO₂ Substrate

Enhanced Electrocatalytic Oxidation of Formate via Introducing Surface Reactive Oxygen Species to a CeO₂ Substrate