Achieving Superior Electrocatalytic Performance by Surface Copper Vacancy Defects during Electrochemical Etching Process

Guo, Niankun; Xue, Hui; Bao, Agula; Wang, Zihong; Sun, Jing; Song, Tianshan; Ge, Xin; Zhang, Wei; Huang, Keke; He, Feng; Wang, Qin

doi:10.1002/anie.202002394

Cited by 167 publications

(101 citation statements)

References 42 publications

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“…In FT-EXAFS spectra of Au L 3 -edge, the peak intensity of np-Cu 1 Au SAA is lower than that of Au foil and np-Au (Fig. 2c), which suggests the formation of lowcoordination Au-Au/Cu defect sites [34,35]. Furthermore, we found that the absorption edge of np-Cu 1 Au SAA is located between the Cu foil and CuO (Fig.…”

Section: Resultsmentioning

confidence: 82%

Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

et al. 2021

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Electrochemical CO 2 reduction is a promising technology for solving the CO 2 emission problems and producing value-added products. Here, we report a hierarchically porous Cu 1 Au single-atom alloy (SAA) as an efficient electrocatalyst for CO 2 reduction. Benefiting from the hierarchically porous architectures with abundant vacancies as well as three-dimensional accessible active sites, the as-prepared nanoporous Cu 1 Au SAA catalyst shows remarkable CO 2 reduction performance with nearly 100% CO Faraday efficiency in a wide potential range (−0.4 to −0.9 V vs. reversible hydrogen electrode. The in-situ X-ray absorption spectroscopy studies and density functional theory calculations reveal that the Cu-Au interface sites serve as the intrinsic active centers, which can facilitate the activated adsorption of CO 2 and stabilize the *COOH intermediate.

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Section: Resultsmentioning

confidence: 82%

Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

et al. 2021

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“…With the reduction of the total noble metals (Pt and Pd) as a key emphasis of the catalyst design while harnessing the above attributes, the third metal, M′, a non-noble transition metal (e.g., Cu, Co, Ni, Fe, etc. ), plays a central role in the catalytic synergy by alloying with the noble metals reflected by optimization of both electronic and strain effects, as known for simple bimetallic systems, e.g., PtCu 31 , and PdCu 32 . Another important consideration of the ternary catalyst design is the exploitation of the increased entropy effect, which is well known to homogenize the compositions towards maximum randomness or remove phase segregation for enhancing corrosion resistance 33 .…”

Section: Resultsmentioning

confidence: 99%

Alloying–realloying enabled high durability for Pt–Pd-3d-transition metal nanoparticle fuel cell catalysts

et al. 2021

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Alloying noble metals with non-noble metals enables high activity while reducing the cost of electrocatalysts in fuel cells. However, under fuel cell operating conditions, state-of-the-art oxygen reduction reaction alloy catalysts either feature high atomic percentages of noble metals (>70%) with limited durability or show poor durability when lower percentages of noble metals (<50%) are used. Here, we demonstrate a highly-durable alloy catalyst derived by alloying PtPd (<50%) with 3d-transition metals (Cu, Ni or Co) in ternary compositions. The origin of the high durability is probed by in-situ/operando high-energy synchrotron X-ray diffraction coupled with pair distribution function analysis of atomic phase structures and strains, revealing an important role of realloying in the compressively-strained single-phase alloy state despite the occurrence of dealloying. The implication of the finding, a striking departure from previous perceptions of phase-segregated noble metal skin or complete dealloying of non-noble metals, is the fulfilling of the promise of alloy catalysts for mass commercialization of fuel cells.

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“…[ 25–30 ] Its structure and its catalytic activity of the shell are revealed to be highly dependent on the used core. [ 31–34 ] This is because the strain effect (expansion or compression) can be effectively controlled, up to the difference of intrinsic lattice parameters between the core and the shell. [ 34–41 ] For example, an expanded strain increases the d‐band center of the active shell, resulting in strengthened adsorption of ethanol and OH species, and eventually much facilitated ethanol electro‐oxidation.…”

Section: Introductionmentioning

confidence: 99%

“…[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.…”

mentioning

confidence: 99%

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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Achieving Superior Electrocatalytic Performance by Surface Copper Vacancy Defects during Electrochemical Etching Process

Cited by 167 publications

References 42 publications

Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

Alloying–realloying enabled high durability for Pt–Pd-3d-transition metal nanoparticle fuel cell catalysts

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

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