Robust copper nanocrystal/nitrogen-doped carbon monoliths as carbon monoxide-resistant electrodes for methanol oxidation reaction

Chen, Fei; Wu, Na; Zhai, Meixu; Zhang, Xue; Guo, Ruihong; Ma, Mingming

doi:10.1016/j.jechem.2020.10.020

Cited by 22 publications

(8 citation statements)

References 41 publications

(47 reference statements)

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“…Furthermore, most of the AOR catalysts are nanomaterials that are loaded on conductive support with the help of binding materials. During long-term AOR at high current densities, the electrical and mechanical contact between conductive support and active catalyst could be easily damaged, which marks a severe decay in the catalytic performance of the electrode 24 , 30 . Therefore, the direct growth of the active catalysts on a conductive substrate to form a monolith electrode is vital for an enhanced AOR performance 31 , 32 .…”

Section: Introductionmentioning

confidence: 99%

In situ grown oxygen-vacancy-rich copper oxide nanosheets on a copper foam electrode afford the selective oxidation of alcohols to value-added chemicals

et al. 2022

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Selective oxidation of low-molecular-weight aliphatic alcohols like methanol and ethanol into carboxylates in acid/base hybrid electrolytic cells offers reduced process operating costs for the generation of fuels and value-added chemicals, which is environmentally and economically more desirable than their full oxidation to CO2. Herein, we report the in-situ fabrication of oxygen-vacancies-rich CuO nanosheets on a copper foam (CF) via a simple ultrasonication-assisted acid-etching method. The CuO/CF monolith electrode enables efficient and selective electrooxidation of ethanol and methanol into value-added acetate and formate with ~100% selectivity. First principles calculations reveal that oxygen vacancies in CuO nanosheets efficiently regulate the surface chemistry and electronic structure, provide abundant active sites, and enhance charge transfer that facilitates the adsorption of reactant molecules on the catalyst surface. The as-prepared CuO/CF monolith electrode shows excellent stability for alcohol oxidation at current densities >200 mA·cm2 for 24 h. Moreover, the abundant oxygen vacancies significantly enhance the intrinsic indicators of the catalyst in terms of specific activity and outstanding turnover frequencies of 5.8k s−1 and 6k s−1 for acetate and formate normalized by their respective faradaic efficiencies at an applied potential of 1.82 V vs. RHE.

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Section: Introductionmentioning

confidence: 99%

In situ grown oxygen-vacancy-rich copper oxide nanosheets on a copper foam electrode afford the selective oxidation of alcohols to value-added chemicals

et al. 2022

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“…Since CO is a poison for many catalysts, the MOR efficiency can be improved by improving the resistance to CO. Therefore, it is very significant to investigate the anti‐CO poisoning ability of catalysts for improving the performance of MOR [35–38] . We put electrodes in a CO‐saturated electrolyte for 15 minute and then compare the LSV curve before and after CO poisoning.…”

Section: Resultsmentioning

confidence: 99%

“…Therefore, it is very significant to investigate the anti-CO poisoning ability of catalysts for improving the performance of MOR. [35][36][37][38] We put electrodes in a CO-saturated electrolyte for 15 minute and then compare the LSV curve before and after CO poisoning. The j value of CPÀ FT-500 catalyst reduced from 352.1 mA/cm 2 to 327.4 mA/cm 2 at 0.6 V, and the j value retention rate was 93 % (Figure 7a).…”

Section: Electrocatalytic Performance For Mormentioning

confidence: 99%

Highly Conductive and CO‐Resistant Cobalt‐Based Monolithic Electrodes for the Catalytic Oxidation of Methanol

Zhai

Chen

et al. 2021

ChemElectroChem

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To develop active and stable electrocatalysts for the methanol oxidation reaction (MOR), many non-noble metal-based nanomaterials have been explored, which are physically loaded on conductive substrates to form electrodes. During a long-term MOR under high current density, these electrodes usually lose activity due to the aggregation or falling off of active nanomaterials. To overcome these problems, we report a simple strategy to synthesize an active, stable, and carbon monoxide (CO)-resistant monolithic electrode for the MOR: cobalt nanocrystal/nitrogen, oxygen-doped carbon (Co@N,OÀ C, CP) monolith. CP monolith shows a high electrical conductivity (1.54 × 10 4 S/cm), which can be directly used as an electrode without any substrate. Co nanocrystals are dispersed uniformly in the N,OÀ C matrix as the active site for MOR, whereas the N,OÀ C matrix protects Co nanocrystals and also facilitates the mass and charge transfer between electrolyte and the electrode. The optimized CPÀ FT-500 electrode presents a high MOR activity of 352 mA/cm 2 at 0.6 V vs SCE (unsaturated calomel electrode) in alkaline electrolyte, which exceeds most previously reported Co-based MOR catalysts. The optimal CPÀ FT-500 catalyst also presents excellent durability and anti-CO poisoning capability (93.3 % retention of activity), which exceeds that of Pt/C (67.5 % retention). Based on its excellent catalytic activity, stability, and high resistance to CO poisoning, CPÀ FT-500 catalyst is a promising low-cost catalyst for MOR.

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“…These supports significantly improve the catalytic performance and stability of the electrocatalyst. In addition, different PVA-PANI Cu/N-C (FT)@500 Electrodeposition 1 M KOH þ 1 M CH 3 OH 189 mA cm À2 0.6 V (vs. SCE) [173] Carbon fiber paper Pd/rGO/CFP Electrodeposition 2 NaOH þ 2 M CH 3 OH 149 mA cm À2 0.9 V (vs. RHE) [176] e-RGO-SWCNT Pt/e-RGO-SWCNT Electrodeposition 0.5 M H 2 SO 4 þ 1 M CH 3 OH197 mA mgPt À1 0.8 V (vs. SCE) [181] functional treatments of these carbon materials can potentially improve their properties. The introduction of heteroatoms can improve electronic properties, promote charge transfer, and provide more active sites.…”

Section: Discussionmentioning

confidence: 99%

“…It can be used as a CO‐resistant MOR electrode with a low cost and good efficiency. [ 173 ] The good mechanical properties and flexibility of polymer films and their ability to conduct protons and electrons give them great potential as catalyst self‐supporting carriers that can be applied to the design and development of a variety of other highly efficient MOR catalysts. However, further development is needed for their successful use as catalyst carriers for commercial DMFC.…”

Section: Self‐supporting Carriersmentioning

confidence: 99%

Review and Development of Anode Electrocatalyst Carriers for Direct Methanol Fuel Cell

Chen

Sun

et al. 2022

Energy Tech

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Direct methanol fuel cell (DMFC) can be used as a promising portable power device due to its excellent energy conversion efficiency and low pollutant emissions. The performance of DMFC largely depends on the anode electrocatalyst for methanol oxidation reaction (MOR). As an important part of the electrocatalyst, the carrier greatly affects the activity and stability of the electrocatalyst. Herein, the research progress of carbonaceous carriers (such as activated carbon, nanostructured carbon), noncarbonaceous carriers (metal compounds), and conducting polymers in DMFC is reviewed. Furthermore, an overview of the development of self‐supporting carriers for flexible DMFC electronics is presented. Its role as the most ideal DMFC carrier in the future provides new ideas for the challenges and development of the commercialization of flexible DMFC.

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Robust copper nanocrystal/nitrogen-doped carbon monoliths as carbon monoxide-resistant electrodes for methanol oxidation reaction

Cited by 22 publications

References 41 publications

In situ grown oxygen-vacancy-rich copper oxide nanosheets on a copper foam electrode afford the selective oxidation of alcohols to value-added chemicals

In situ grown oxygen-vacancy-rich copper oxide nanosheets on a copper foam electrode afford the selective oxidation of alcohols to value-added chemicals

Highly Conductive and CO‐Resistant Cobalt‐Based Monolithic Electrodes for the Catalytic Oxidation of Methanol

Review and Development of Anode Electrocatalyst Carriers for Direct Methanol Fuel Cell

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