In Situ Raman Study of CO Electrooxidation on Pt(<i>hkl</i>) Single‐Crystal Surfaces in Acidic Solution

Su, Min; Dong, Jin‐Chao; Le, Jia‐Bo; Zhao, Yu; Yang, Weimin; Yang, Zhilin; Attard, Gary Anthony; Liu, Guokun; Cheng, Jun; Wei, Yimin; Zhang, Tian; Li, Jianfeng

doi:10.1002/anie.202010431

Cited by 56 publications

(43 citation statements)

References 52 publications

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“…The difference of this oxidation process on these catalysts confirms varied adsorption capability of CO on these catalysts. [52] Such a statement is further supported by the adsorption/desorption behavior of hydrogen on these catalysts. No clear waves are seen with respect to hydrogen adsorption/desorption once the surfaces of the Pt nanoparticles, the PdPt alloy, and the Au@ PdPt core-shell catalyst are saturated with CO. Once the COstripping experiment is conducted, the waves of hydrogen adsorption/desorption (left side of the dash lines, red curves in Figure 3a) are clearly seen on these catalysts.…”

Section: Aor Performance On the Au@pdpt Core-shell Catalystmentioning

confidence: 77%

Modulating Electronic Structure of an Au‐Nanorod‐Core–PdPt‐Alloy‐Shell Catalyst for Efficient Alcohol Electro‐Oxidation

Yang

Wang

Qing

et al. 2021

Advanced Energy Materials

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are more convenient and secure to be transported and stored. However, the conversion efficiencies of these AORs are commonly inferior to hydrogen oxidation. This is partially due to the sluggish kinetics of multielectrons' transferred processes inside alcohols (e.g., methanol, ethanol, ethylene glycol, and glycerol). [7][8][9][10][11] In this regard, various catalysts of both noble and non-noble metals have been designed and synthesized to boost such sluggish AORs. Although noble metal catalysts (e.g., Pd, Pt, and Rh) are more expensive than non-noble metals (e.g., Ni, Co, and Mn), their more negative AOR onset potentials make them superior for the construction of DAFCs, [4,5,11] originating from their unique electronic structures. Among reported noble-based catalysts, those based on the Pt metal are regarded as the star electrocatalysts for the AORs in terms of their oxidation overpotentials and Tafel slopes. [12,13] Notably, their alloys with other metals (e.g., Ru, Ni, Co, Pd, Rh, and Au) exhibit strong adsorption capability toward OH species or a so-called bifunctional mechanism, leading to improved AOR performance. [14][15][16][17] On the other hand, the serious poisoning effect of the carbonaceous intermediates (especially CO) hinders dramatically the activity of the used catalysts (especially the Pt catalysts) and eventually leads to much reduced conversion efficiencies of the AORs. [18,19] In this context, the screwlike PdPt alloy nanowires [19] and PdPt alloy nanoparticles [20] have been employed to replace single metallic Pt catalysts for methanol electro-oxidation reaction (MOR). Originating from varied electronic structures that are induced by the addition of Pd atoms, these PdPt alloys have been confirmed as commendable MOR catalysts. Although the sizes and compositions of these catalysts have been tuned and the AOR performance on these catalysts has been explored, the performance of these bimetallic heterostructures/catalysts is still far away for their commercial applications. The catalysts featuring superior AOR performance over those reported are still highly demanded for the construction of high-performance DAFCs.It has been well known that the optimization of these noble-metallic heterostructures/catalysts with respect to their morphologies and exposed facets is helpful to enhance their catalytic performance. [21][22][23][24] Among various heterostructures, a catalyst with a core-shell structure has been attracted special attention. [25][26][27][28][29][30] Its structure and its catalytic activity of the shell are revealed to be highly dependent on the used core. [31][32][33][34] This is because the strain effect (expansion or compression) can be Direct alcohol fuel cells (DAFCs) utilize alcohol electro-oxidation reactions (AORs) to provide electricity, where catalysts with optimal electronic structures are required to accelerate sluggish AORs. Herein, an electrocatalyst with an Au-nanorod core and a PdPt-alloy shell is designed. Its electronic structures are modulated through epitaxial growth ...

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Section: Aor Performance On the Au@pdpt Core-shell Catalystmentioning

confidence: 77%

Modulating Electronic Structure of an Au‐Nanorod‐Core–PdPt‐Alloy‐Shell Catalyst for Efficient Alcohol Electro‐Oxidation

Yang

Wang

Qing

et al. 2021

Advanced Energy Materials

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“…In contrast with the stable atoms in the grain, the atoms around the stepped surface and vacancies are usually in the metastable state of unsaturated coordination number, which can further provide unique adsorption capacity for *COOH [37–39] . Numerous in situ experiments have been carried out to study the types of CO 2 RR intermediates and their adsorption strength [40–43] . Alternatively, electrochemical analysis was also performed to directly verify the adsorption strength of reactive intermediates.…”

Section: Resultsmentioning

confidence: 99%

Enhanced Electrochemical Reduction of CO₂to CO on Ag/SnO₂by a Synergistic Effect of Morphology and Structural Defects

Wang

et al. 2021

Chemistry An Asian Journal

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Silver (Ag)‐based materials are considered to be promising materials for electrochemical reduction of CO2 to produce CO, but the selectivity and efficiency of traditional polycrystalline Ag materials are insufficient; there still exists a great challenge to explore novel modified Ag based materials. Herein, a nanocomposite of Ag and SnO2 (Ag/SnO2) for efficient reduction of CO2 to CO is reported. HRTEM and XRD patterns clearly demonstrated the lattice destruction of Ag and the amorphous SnO2 in the Ag/SnO2 nanocomposite. Electrochemical tests indicated the nanocomposite containing 15% SnO2 possesses highest catalytic selectivity featured by a CO faradaic efficiency (FE) of 99.2% at −0.9 V versus reversible hydrogen electrode (vs RHE) and FE>90% for the CO product at a wide potential range from −0.8 V to −1.4 V vs RHE. Experimental characterization and analysis showed that the high catalytic performance is attributed to not only the branched morphology of Ag/SnO2 nanocomposites (NCs), which endows the maximum exposure of active sites, but also the special adsorption capacity of abundant defect sites in the crystal for *COOH (the key intermediate of CO formation), which improves the intrinsic activity of the catalyst. But equally important, the existed SnO2 also plays an important role in inhibiting hydrogen evolution reaction (HER) and anchoring defect sites. This work demonstrates the use of crystal defect engineering and synergy in composite to improve the efficiency of electrocatalytic CO2 reduction reaction (CO2RR).

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“…Understanding the adsorption and oxidation of CO molecules is an important step in designing enhanced catalysts. According to previous studies [ 65 ], the Co electrooxidation reaction occurs through a surface bimolecular reaction in which the CO* and OH* intermediates adsorbed on the catalyst surface participate in the formation of COOH* intermediates, as shown in Fig. 8 a.…”

Section: Carbon Monoxide Oxidation Reactionmentioning

confidence: 92%

“…SHINERS has been used to gain mechanistic insights into various electrochemical reactions, including HER [ 21 , 44 ], ORR [ 20 , 48 ], CO reduction reaction (CORR) [ 15 , 47 ], CO oxidation reaction (COOR) [ 64 , 65 ], CO adsorption [ 44 ], OER [ 46 ], and NO 3 RR [ 50 ]. Table 1 summarizes the applications of SHINERS in the electrocatalysis research field, as well as the detailed experimental conditions, such as SHINs, electrode, electrolyte, and laser wavelength.…”

Section: Shiners Applicationmentioning

confidence: 99%

Shell isolated nanoparticle enhanced Raman spectroscopy for mechanistic investigation of electrochemical reactions

Haryanto

Lee

2022

Nano Convergence

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Electrochemical conversion of abundant resources, such as carbon dioxide, water, nitrogen, and nitrate, is a remarkable strategy for replacing fossil fuel-based processes and achieving a sustainable energy future. Designing an efficient and selective electrocatalysis system for electrochemical conversion reactions remains a challenge due to a lack of understanding of the reaction mechanism. Shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) is a promising strategy for experimentally unraveling a reaction pathway and rate-limiting step by detecting intermediate species and catalytically active sites that occur during the reaction regardless of substrate. In this review, we introduce the SHINERS principle and its historical developments. Furthermore, we discuss recent SHINERS applications and developments for investigating intermediate species involved in a variety of electrocatalytic reactions.

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In Situ Raman Study of CO Electrooxidation on Pt(hkl) Single‐Crystal Surfaces in Acidic Solution

Cited by 56 publications

References 52 publications

Modulating Electronic Structure of an Au‐Nanorod‐Core–PdPt‐Alloy‐Shell Catalyst for Efficient Alcohol Electro‐Oxidation

Modulating Electronic Structure of an Au‐Nanorod‐Core–PdPt‐Alloy‐Shell Catalyst for Efficient Alcohol Electro‐Oxidation

Enhanced Electrochemical Reduction of CO₂to CO on Ag/SnO₂by a Synergistic Effect of Morphology and Structural Defects

Shell isolated nanoparticle enhanced Raman spectroscopy for mechanistic investigation of electrochemical reactions

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In Situ Raman Study of CO Electrooxidation on Pt(hkl) Single‐Crystal Surfaces in Acidic Solution

Cited by 56 publications

References 52 publications

Modulating Electronic Structure of an Au‐Nanorod‐Core–PdPt‐Alloy‐Shell Catalyst for Efficient Alcohol Electro‐Oxidation

Modulating Electronic Structure of an Au‐Nanorod‐Core–PdPt‐Alloy‐Shell Catalyst for Efficient Alcohol Electro‐Oxidation

Enhanced Electrochemical Reduction of CO2to CO on Ag/SnO2by a Synergistic Effect of Morphology and Structural Defects

Shell isolated nanoparticle enhanced Raman spectroscopy for mechanistic investigation of electrochemical reactions

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Enhanced Electrochemical Reduction of CO₂to CO on Ag/SnO₂by a Synergistic Effect of Morphology and Structural Defects