Cobalt‐Doping Stabilized Active and Durable Sub‐2 nm Pt Nanoclusters for Low‐Pt‐Loading PEMFC Cathode (Adv. Energy Mater. 13/2022)

Duan, Xiao; Cao, Feng; Ding, Rui; Li, Xiaoke; Li, Qingbing; Aisha, Ruziguli; Zhang, Shiqiao; Ke, Hua; Rui, Zhiyan; Wu, Yongkang; Li, Jia; Li, Aidong; Liu, Jianguo

doi:10.1002/aenm.202270055

Cited by 12 publications

(19 citation statements)

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“…Consequently, the outstanding stability of the Co‐Rh 2 electrocatalyst stems from that Co doping reduces the total energy required to stabilize the nanoparticles. [ 51 ]…”

Section: Resultsmentioning

confidence: 99%

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co‐Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Guo

Yang

Liu

et al. 2022

Adv Funct Materials

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Efficient hydrogen production from electrochemical overall water splitting requires high‐performance electrocatalysts for hydrogen evolution reaction (HER) and a fast oxidation reaction to replace sluggish oxygen evolution reaction. Herein, Co‐doped Rh nanoparticles are thus grown on carbon black using Co nanosheets as the bridge. These nanoparticles with a size of ≈1.94 nm exhibit the overpotential of as low as 2 mV at 10 mA cm−2 for the HER, and a mass activity of as high as 889 mA mg−1 for the methanol oxidation reaction (MOR) in alkaline media. As confirmed by density functional theory simulations, such excellent activity originates from Co‐doping, which reduces reaction energy barriers for both the rate‐determining step of a Volmer process during the HER and the conversion of *CO to COOH* during the MOR (namely the enhanced adsorption of H2O and COOH*). Coupling boosted HER on the cathode with accelerated MOR on the anode, efficient H2 generation is achieved. This two‐electrode cell only requires a cell voltage of 1.545 V at 10 mA cm−2 with impressive long‐life cycling stability. Such performance even outperforms that of commercial Pt/C || IrO2 cell. This study offers a new strategy to achieve efficient HER from overall water splitting.

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“…Consequently, the outstanding stability of the Co‐Rh 2 electrocatalyst stems from that Co doping reduces the total energy required to stabilize the nanoparticles. [ 51 ]…”

Section: Resultsmentioning

confidence: 99%

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co‐Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Guo

Yang

Liu

et al. 2022

Adv Funct Materials

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“…[ 36 ] For the Pt 4f state in PtCo NCs/N–CNTs‐900 in Figure S7b (Supporting Information), the lower ratio of the metallic Pt state suggests the absence of a single atom Pt and a possible durability decrease. [ 37 ] As revealed in Figure 2h and Figure S7c (Supporting Information), The C 1s spectrum for Pt SA –PtCo NCs/N–CNTs‐900 and PtCo NCs/N–CNTs‐900 exhibits three peaks, associated with graphitic C═C, C─N, and C─O, respectively. For the N 1s spectra shown in Figure 2i, there are five peaks located at 398.5, 399.2, 400.4, 401.5, and 403.6 eV, which correspond to the pyridinic N, Co─N x , pyrrolic N, graphitic N, and oxidized N states, respectively.…”

Section: Resultsmentioning

confidence: 98%

Neighboring Platinum Atomic Sites Activate Platinum–Cobalt Nanoclusters as High‐Performance ORR/OER/HER Electrocatalysts

Chen

Zhu

Wei

et al. 2023

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The rational design of efficient and multifunctional electrocatalysts for energy conversion devices is one of the major challenges for clean and renewable energy transition. Herein, the local electronic structure of cobalt–platinum nanoclusters is regulated by adjacent platinum atomic site encapsulated in N‐doped hollow carbon nanotubes (PtSA–PtCo NCs/N–CNTs) by pyrolysis of melamine‐orientation‐induced zeolite imidazole metal–organic frameworks (ZIF‐67) with thimbleful platinum doping. The introduction of melamine can reactivate adjacent carbon atoms and initiate the oriented growth of nitrogen‐doped carbon nanotubes. The systematic analysis suggests the significant role of thimbleful neighboring low‐coordinated Pt─N2 in altering the localized electronic structure of PtCo nanoclusters. The optimized PtSA–PtCo NCs/N–CNTs‐900 exhibit excellent hydrogen evolution reaction (HER)/oxygen evolution reaction (OER)/oxygen reduction reaction (ORR)/ catalytic performance reaching the current density of 10 mA cm−2 in 1 m KOH under the low 47 (HER) and 252 mV (OER) overpotentials, and a high half‐wave potential of 0.86 and 0.89 V (ORR) in 0.1 m KOH and 0.1 m HClO4, respectively. Remarkably, the PtSA–PtCo NC/N–CNT‐900 also presents outstanding catalytic performances toward water splitting and rechargeable Zn–air batteries. The theoretical calculations reveal that optimal regulation of the electronic structure of PtCo nanoclusters by thimbleful neighboring Pt atomic reduces the reaction energy barrier in electrochemical process, facilitating the ORR/OER/HER performance.

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“…and further precisely tuning its composition and structure. [ 4–14 ] It is reported that structurally ordered intermetallic Pt–M alloys exhibited a significant enhancement on ORR performance. The enhanced performance is attributed to that incorporating M atoms with a smaller atomic radius in the Pt–M alloys provides a compressive strain to Pt atoms on the surface, lowers its d‐band center, and further weakens the O 2 /intermediates adsorption, which is the rate‐determining step of ORR.…”

Section: Introductionmentioning

confidence: 99%

Electronic Enhancement Engineering by Atomic Fe–N₄ Sites for Highly‐Efficient PEMFCs: Tailored Electric‐Thermal Field on Pt Surface

Wang

Yang

Wang

et al. 2023

Advanced Energy Materials

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Fortunately, proton exchange membrane fuel cells (PEMFCs) possess the potential of higher energy densities depending on the amount of carried H 2 , which have realized the commercial application in the field of heavy truck and shipping. Oxygen reduction reaction (ORR) is the cathode reaction of PEMFCs. [1][2] Its sluggish kinetics directly hinder the overall efficiency of PEMFCs. Although commercial carbon supported Pt (Pt/C) has been proven to be the most efficient electrocatalysts for ORR, their scarcity, high cost, and poor stability in long-term operations is a huge impediment to the large-scale deployment of PEMFCs. [3] To address these issues, it is urgently needed to reduce the Pt usage simultaneously improving its activity and stability, or ultimately to replace precious metal Ptbased catalysts with non-precious-metal catalysts.An effective strategy to reduce Pt usage is alloying Pt with a second transition metal (M = Fe, Co, Ni, etc.) and further precisely tuning its composition and structure. [4][5][6][7][8][9][10][11][12][13][14] It is reported that structurally ordered intermetallic Pt-M alloys exhibited a significant enhancement on ORR performance. The enhanced performance is attributed to that incorporating M atoms with a smaller atomic radius in the Pt-M alloys provides a compressive strain to Pt atoms on the surface, lowers its d-band center, Lowering noble-metal Pt usage and simultaneously enhancing electrocatalytic oxygen reduction reaction (ORR) activity and stability of Pt-based ORR electrocatalysts is the key to realize the large-scale application of fuel cells. Here, an effective strategy is developed to reduce Pt usage through the strong electron interaction between uniform Pt nanoparticles (≈4.0 nm) and abundant atomically dispersed Fe-N 4 sites modified on an ordered mesoporous carbon (OMC) surface for efficiently enhancing ORR performance. Density functional theory (DFT) calculations show that the strong electron interactions between Pt and Fe-N 4 sites decrease the d-band center of Pt in Pt@Fe-N-OMC-2 by 0.21 eV relative to that of as-prepared Pt@OMC, indicating the weakened O 2 adsorption and accelerated desorption of oxygenated species on Pt sites. In situ Raman spectra demonstrate that the introduction of Fe-N 4 moieties promotes the O-OH dissociation process. Finite element method simulations reveal that the electric and thermal field of the embedded Pt nanoparticle surface is enhanced through modifying Fe-N 4 sites on the OMC surface, accelerating the accumulation of ORR-related species (O 2 , H + , and H 2 O), which is conductive to electrocatalyzing the ORR. This innovative approach not only illustrates the synergistic mechanism between Pt and Fe-N 4 sites, but also simultaneously provides new avenues to design advanced electrocatalysts for fuel cells.

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Cobalt‐Doping Stabilized Active and Durable Sub‐2 nm Pt Nanoclusters for Low‐Pt‐Loading PEMFC Cathode (Adv. Energy Mater. 13/2022)

Cited by 12 publications

References 0 publications

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co‐Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co‐Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Neighboring Platinum Atomic Sites Activate Platinum–Cobalt Nanoclusters as High‐Performance ORR/OER/HER Electrocatalysts

Electronic Enhancement Engineering by Atomic Fe–N₄ Sites for Highly‐Efficient PEMFCs: Tailored Electric‐Thermal Field on Pt Surface

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Cobalt‐Doping Stabilized Active and Durable Sub‐2 nm Pt Nanoclusters for Low‐Pt‐Loading PEMFC Cathode (Adv. Energy Mater. 13/2022)

Cited by 12 publications

References 0 publications

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co‐Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Coupling Methanol Oxidation with Hydrogen Evolution on Bifunctional Co‐Doped Rh Electrocatalyst for Efficient Hydrogen Generation

Neighboring Platinum Atomic Sites Activate Platinum–Cobalt Nanoclusters as High‐Performance ORR/OER/HER Electrocatalysts

Electronic Enhancement Engineering by Atomic Fe–N4 Sites for Highly‐Efficient PEMFCs: Tailored Electric‐Thermal Field on Pt Surface

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Electronic Enhancement Engineering by Atomic Fe–N₄ Sites for Highly‐Efficient PEMFCs: Tailored Electric‐Thermal Field on Pt Surface