Oxygen vacancies endow atomic cobalt-palladium oxide clusters with outstanding oxygen reduction reaction activity

Yang, Thomas C.-K.; Bhalothia, Dinesh; Chang, Hsiu-Ju; Yan, Che; Beniwal, Amisha; Chang, You-Xun; Wu, Shun-Chi; Chen, Po-Chun; Wang, Kuan Wen; Dai, Sheng; Chen, Tsan‐Yao

doi:10.1016/j.cej.2022.140289

Cited by 13 publications

(10 citation statements)

References 53 publications

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“…Considering that no charge transfer for the 1Pd/ catalyst was measured, for which Pd is exclusively on titania, and considering the BE of Pd and Co, a charge transfer occurs from cobalt oxide to Pd due to electronegativity difference and lattice strain. 75 This result suggests that a significant portion of Pd should be located on cobalt in the 1Pd–10Co-o/ catalyst.…”

Section: Resultsmentioning

confidence: 97%

Effects of Pd and Co intimacy in Pd-modified Co/TiO₂ catalysts for direct CO₂ hydrogenation to fuels: the closer not the better

Scarfiello,

Durupt,

Tison

et al. 2024

Catal. Sci. Technol.

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Section: Resultsmentioning

confidence: 97%

Effects of Pd and Co intimacy in Pd-modified Co/TiO₂ catalysts for direct CO₂ hydrogenation to fuels: the closer not the better

Scarfiello,

Durupt,

Tison

et al. 2024

Catal. Sci. Technol.

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“…On top of that, the cobalt oxide support supplies the electrons to surface Pd-sites. [108] In addition to noble metal catalysts, transition metal-based catalysts are also frequently reported for this case. For example, Wei et al reported that the co-presence of Zn single atoms, clusters and nanoparticles embedded into hybrid carbon aerogels (denoted as Zn/NC) shows a fascinating ORR performance and achieved the half-wave potential of 0.845 V. [109]…”

Section: Local Synergy Between Single Atoms Atomic Clusters and Nanop...mentioning

confidence: 92%

Bridging the Gap Between Single Atoms, Atomic Clusters and Nanoparticles in Electrocatalysis: Hierarchical Structured Heterogeneous Catalysts

Bhalothia,

Beniwal,

Kumar Saravanan

et al. 2024

ChemElectroChem

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In the past decade, remarkable progress has been made in advancing heterogeneous single‐atom catalysts (SACs), propelled by their extraordinary properties such as unique activities, high selectivity, and efficient metal utilization. In contrast to their nanoparticle counterparts, SACs showcase distinct advantages, yet they are not exempt from limitations. A primary constraint lies in their relatively low metal content and lack of ensemble sites, potentially impacting overall catalytic activity. Stability concerns also arise, as isolated metal atoms may be prone to aggregation, oxidation, and other structural changes. To surmount these challenges, there is a burgeoning exploration of synergies between SACs and other active species, such as single atoms, atomic clusters, or nanoparticles. This approach holds promise for augmenting the efficiency of complex catalytic reactions. However, a systematic examination of their integration and potential synergy has been notably absent. This review strives to fill that gap by comprehensively exploring key interactions, complementary effects, and bifunctional roles of single atoms, atomic clusters and nanoparticles when combined in different compositions and configurations, especially for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) applications. Additionally, the review sheds new light on the underlying catalytic mechanisms by offering insights through specific case studies. In particular, it emphasizes the dynamic nature of each active species and their interactions within these innovative catalytic entities, specifically in the context of heterogeneous electrocatalytic processes, backed by compelling in situ and operando evidence. Concluding the discussion, the review addresses the current challenges and provides a glimpse into the prospects of these integrated catalytic systems in the future. The contents can serve as a valuable guide for the design of advanced catalysts, promoting the deliberate combination and synergy of binary or multiple active species to further advance the field of catalysis with a clear roadmap and easy assessments.

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“…Figure 4 shows the CO stripping curves of CoPd, CoPd-1, and CoPd-10 samples compared with the control samples (Pd-AC and Co-AC). Accordingly, the nearly flattened current responses for AC-supported Co NPs (i.e., the Co-AC) suggested their inert behaviour towards CO molecules [23]. Meanwhile, the AC-supported Pd NPs (i.e., Pd-AC) exhibited a sharp CO-oxidation peak (P) at ~0.955 V vs. NHE, which corresponded to the CO-oxidation from the closely packed (111) facet.…”

Section: Structural Properties Of Copd Nanocatalystsmentioning

confidence: 98%

“…Figure 2a shows the X-ray absorption near-edge spectroscopy (XANES) spectra of pristine and laser-irradiated CoPd nanocatalysts, while the XANES spectra of standard Co foil and CoO were compared for reference. The XANES spectra at Co K-edge showed three main regions, including the pre-edge "R", the position of the inflection point (I S ), and the intensity of the absorption edge (or whiteline) (H S ), which, respectively, corresponded to the local geometry around the Co atoms, the oxidation state, and the extent of occupied/unoccupied state (due to electronic interaction with neighbouring atoms) of the targeting atom [23,24]. As shown in Figure 2a, the CoPd, CoPd-1, and CoPd-10 nanocatalysts exhibited similar features in all three regions, suggesting the unchanged local atomic and electronic properties of CoOx in CoPd after laser irradiation.…”

Section: Structural Properties Of Copd Nanocatalystsmentioning

confidence: 99%

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Sub-Millisecond Laser-Irradiation-Mediated Surface Restructure Boosts the CO Production Yield of Cobalt Oxide Supported Pd Nanoparticles

et al. 2023

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The catalytic conversion of CO2 into valuable commodities has the potential to balance ongoing energy and environmental issues. To this end, the reverse water–gas shift (RWGS) reaction is a key process that converts CO2 into CO for various industrial processes. However, the competitive CO2 methanation reaction severely limits the CO production yield; therefore, a highly CO-selective catalyst is needed. To address this issue, we have developed a bimetallic nanocatalyst comprising Pd nanoparticles on the cobalt oxide support (denoted as CoPd) via a wet chemical reduction method. Furthermore, the as-prepared CoPd nanocatalyst was exposed to sub-millisecond laser irradiation with per-pulse energies of 1 mJ (denoted as CoPd-1) and 10 mJ (denoted as CoPd-10) for a fixed duration of 10 s to optimize the catalytic activity and selectivity. For the optimum case, the CoPd-10 nanocatalyst exhibited the highest CO production yield of ∼1667 μmol g−1catalyst, with a CO selectivity of ∼88% at a temperature of 573 K, which is a 41% improvement over pristine CoPd (~976 μmol g−1catalyst). The in-depth analysis of structural characterizations along with gas chromatography (GC) and electrochemical analysis suggested that such a high catalytic activity and selectivity of the CoPd-10 nanocatalyst originated from the sub-millisecond laser-irradiation-assisted facile surface restructure of cobalt oxide supported Pd nanoparticles, where atomic CoOx species were observed in the defect sites of the Pd nanoparticles. Such an atomic manipulation led to the formation of heteroatomic reaction sites, where atomic CoOx species and adjacent Pd domains, respectively, promoted the CO2 activation and H2 splitting steps. In addition, the cobalt oxide support helped to donate electrons to Pd, thereby enhancing its ability of H2 splitting. These results provide a strong foundation to use sub-millisecond laser irradiation for catalytic applications.

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Oxygen vacancies endow atomic cobalt-palladium oxide clusters with outstanding oxygen reduction reaction activity

Cited by 13 publications

References 53 publications

Effects of Pd and Co intimacy in Pd-modified Co/TiO₂ catalysts for direct CO₂ hydrogenation to fuels: the closer not the better

Effects of Pd and Co intimacy in Pd-modified Co/TiO₂ catalysts for direct CO₂ hydrogenation to fuels: the closer not the better

Bridging the Gap Between Single Atoms, Atomic Clusters and Nanoparticles in Electrocatalysis: Hierarchical Structured Heterogeneous Catalysts

Sub-Millisecond Laser-Irradiation-Mediated Surface Restructure Boosts the CO Production Yield of Cobalt Oxide Supported Pd Nanoparticles

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Oxygen vacancies endow atomic cobalt-palladium oxide clusters with outstanding oxygen reduction reaction activity

Cited by 13 publications

References 53 publications

Effects of Pd and Co intimacy in Pd-modified Co/TiO2 catalysts for direct CO2 hydrogenation to fuels: the closer not the better

Effects of Pd and Co intimacy in Pd-modified Co/TiO2 catalysts for direct CO2 hydrogenation to fuels: the closer not the better

Bridging the Gap Between Single Atoms, Atomic Clusters and Nanoparticles in Electrocatalysis: Hierarchical Structured Heterogeneous Catalysts

Sub-Millisecond Laser-Irradiation-Mediated Surface Restructure Boosts the CO Production Yield of Cobalt Oxide Supported Pd Nanoparticles

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Product

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Effects of Pd and Co intimacy in Pd-modified Co/TiO₂ catalysts for direct CO₂ hydrogenation to fuels: the closer not the better

Effects of Pd and Co intimacy in Pd-modified Co/TiO₂ catalysts for direct CO₂ hydrogenation to fuels: the closer not the better