Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene

Xiong, Yu; Sun, Wenming; Han, Yunhu; Xin, Pingyu; Zheng, Xusheng; Yan, Wensheng; Dong, Juncai; Zhang, Jian; Wang, Dingsheng; Li, Yadong

doi:10.1007/s12274-020-3244-4

Cited by 279 publications

(139 citation statements)

References 57 publications

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“…The development of highly active and low-cost electrocatalysts for the ethanol oxidation reaction (EOR) lays at the heart of DEFCs 16 – 25 . Down-sizing of metal nanoparticles into individual metal sites is commonly regarded as an efficient approach to enhance the performance and cost-effectiveness of electrocatalysts, but may be improper for specific reactions catalyzed by multiple sites or peculiar active centers 26 – 31 . For now, alloying of Pd with base metals (M) like Zn, Ni, Sn, Co, Cu, Ge, etc.…”

Section: Introductionmentioning

confidence: 99%

Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction

et al. 2021

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Rational design and synthesis of superior electrocatalysts for ethanol oxidation is crucial to practical applications of direct ethanol fuel cells. Here, we report that the construction of Pd-Zn dual sites with well exposure and uniformity can significantly improve the efficiency of ethanol electro-oxidation. Through synthetic method control, Pd-Zn dual sites on intermetallic PdZn nanoparticles, Pd-Pd sites on Pd nanoparticles and individual Pd sites are respectively obtained on the same N-doped carbon coated ZnO support. Compared with Pd-Pd sites and individual Pd sites, Pd-Zn dual sites display much higher activity for ethanol electro-oxidation, exceeding that of commercial Pd/C by a factor of ~24. Further computational studies disclose that Pd-Zn dual sites promote the adsorption of ethanol and hydroxide ion to optimize the electro-oxidation pathway with dramatically reduced energy barriers, leading to the superior activity. This work provides valuable clues for developing high-performance ethanol electro-oxidation catalysts for fuel cells.

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Section: Introductionmentioning

confidence: 99%

Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction

et al. 2021

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“…As shown in Fig. 2(g), the N 1s XPS for the two samples can be fitted into three main components including pyridinic-N (398.4 eV), Mn-N (399.1 eV) and graphitic-N (401.1 eV) [34,35]. Moreover, the percentage of Mn-N was increased after the NH 3 reparing step.…”

Section: Resultsmentioning

confidence: 86%

Structural revolution of atomically dispersed Mn sites dictates oxygen reduction performance

et al. 2021

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An efficient preparation and local coordination environment regulation of isolated single-atom sites catalysts (ISASC) for improved activity is still challenging. Herein, we develop a solid phase thermal diffusion strategy to synthesize Mn ISASC on highly uniform nitrogen-doped carbon nanotubes by employing MnO 2 nanowires@ZIF-8 core-shell structure. Under hightemperature, the Mn species break free from core-MnO 2 lattice, which will be trapped by carbon defects derived from shell-ZIF-8 carbonization, and immobilized within carbon substrate. Furthermore, the poly-dispersed Mn sites with two nitrogen-coordinated centers can be controllably renovated into four-nitrogen-coordinated Mn sites using NH 3 treatment technology. Both experimental and computational investigations indicate that the symmetric coordinated Mn sites manifest outstanding oxygen reduction activity and superior stability in alkaline and acidic solutions. This work not only provides efficient way to regulate the coordination structure of ISASC to improve catalytic performance but also paves the way to reveal its significant promise for commercial application.

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“…However, there is still some barrier on the way to apply the SACs in the practical hydrogen production [34, 35] . To realize the practical use of the single atomic site catalysts, several problems are needed to be considered, such as regulating the catalytic efficiency of metallic center, regulating the conductivity of basement and so on [36–42] . The interaction between metallic center and basement has also been noticed for a long time [43–45] .…”

Section: Figurementioning

confidence: 99%

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

et al. 2021

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It is still of great difficulty to develop the non‐platinum catalyst with high catalytic efficiency towards hydrogen evolution reaction via the strategies till now. Therefore, it is necessary to develop the new methods of catalyst designing. Here, we put forward the catalyst designed by the electronic metal–support interaction (EMSI), which is demonstrated to be a reliable strategy to find out the high‐efficiency catalyst. We carried out the density functional theory calculation first to design the proper EMSI of the catalyst. We applied the model of M1‐M2‐X (X=C, N, O) during the calculation. Among the catalysts we chose, the EMSI of Rh1TiC, with the active sites of Rh1‐Ti2C2, is found to be the most proper one for HER. The electrochemical experiment further demonstrated the feasibility of the EMSI strategy. The single atomic site catalyst of Rh1‐TiC exhibits higher catalytic efficiency than that of state‐of‐art Pt/C. It achieves a small overpotential of 22 mV and 86 mV at the at the current density of 10 mA cm−2 and 100 mA cm−2 in acid media, with a Tafel slope of 25 mV dec−1 and a mass activity of 54403.9 mA cm−2 mgRh−1 (vs. 192.2 mA cm−2 mgPt−1 of Pt/C). Besides, it also shows appealing advantage in energy saving compared with Pt/C (≈20 % electricity consuming decrease at 2 kA m−2) Therefore, we believe that the strategy of regulating EMSI can act as a possible way for achieving the high catalytic efficiency on the next step of SACs.

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Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene

Cited by 279 publications

References 57 publications

Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction

Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction

Structural revolution of atomically dispersed Mn sites dictates oxygen reduction performance

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

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