Understanding catalytic activity trends of atomic pairs in single-atom catalysts towards oxygen reduction reactions

Zhang, Fengchu; Xie, Weiwei; Zhang, Na; Li, Sha; Wang, Xi

doi:10.1016/j.apsusc.2022.153873

Cited by 4 publications

(4 citation statements)

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“…Figure a shows the position of doped atoms as well as the detailed coordination environment of TM 1 and adjacent Ti atoms. Based on our previous study, the atomically dispersed TM dopants bind strongly in TM 1 @TiO 2 nanosheets with significant negative binding energies, implying the good stability of TM 1 @TiO 2 nanosheets during HER . Particularly, Ru 1 @TiO 2 nanosheets maintain excellent HER activity after four consecutive HER cycles (24 h) in neutral media .…”

Section: Resultsmentioning

confidence: 99%

“…Based on our previous study, the atomically dispersed TM dopants bind strongly in TM 1 @TiO 2 nanosheets with significant negative binding energies, implying the good stability of TM 1 @TiO 2 nanosheets during HER. 38 Particularly, Ru 1 @TiO 2 nanosheets maintain excellent HER activity after four consecutive HER cycles (24 h) in neutral media. 22 To screen suitable catalysts for H 2 production, we evaluated a total of 14 TM 1 @TiO 2 systems based on three criteria (Figure 1b).…”

Section: Catalyst Models and Screening Rulesmentioning

confidence: 99%

“…According to our previous study on TiO 2 nanosheets, there is no strong correlation between the d-band center of the active site Ti or TM and the energy of OH. 38 In addition, we plot the scaling relationship between the d-band filling of TM or Ti atom and G *OH , and the results (R 2 = 0.77 and 0.26) show that the d-band filling could not serve as an effective descriptor for G *OH in neutral HER (Figure S6 and Tables S8 and S9). Electronic density of state (DOS) plot shows that impurity energy levels of TM 1 @TiO 2 nanosheets divide the large band gap region into several small parts (Figures 5a,b and S7).…”

Section: Deep Mechanism Analysis At the Orbital-scalementioning

confidence: 99%

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Orbital Orientation-based Theoretical Design of Single-Atom Catalysts for the Hydrogen Evolution Reaction

Zhang

Ding

et al. 2022

J. Phys. Chem. C

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Hydrogen evolution reaction (HER) is regarded as one of the most effective routes to produce H2, but it usually suffers from the lack of the novel design concept of high-efficiency catalysts, especially in neutral condition. Herein, we report an orbital orientation-based theoretical principle for designing efficient single-atom HER catalysts. Through screening 14 catalysts consisting of the transition-metal single atoms doped into TiO2 (TM1@TiO2) nanosheets, we demonstrate that the d orbital orientation of TM1–Ti1 atomic pairs plays a key role in the regulation of catalytic activities. Among them, Pd1@TiO2 is screened out as an excellent HER catalyst in neutral media, where the Pd- orbital tends to be exposed due to the existence of Pd1–Ti1 atomic pair and thus promotes OH desorption and the overall hydrogen production. This work provides a new insight through tailoring high-performance orbital catalysts and sheds an orbital-level understanding of the HER mechanism.

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Section: Resultsmentioning

confidence: 99%

Section: Catalyst Models and Screening Rulesmentioning

confidence: 99%

Section: Deep Mechanism Analysis At the Orbital-scalementioning

confidence: 99%

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Orbital Orientation-based Theoretical Design of Single-Atom Catalysts for the Hydrogen Evolution Reaction

Zhang

Ding

et al. 2022

J. Phys. Chem. C

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“…In this way, not only can Pt compressive strain be controlled precisely, but also unexpected effects of ligands or heteroatoms can be avoided. [37][38][39] As a result, a convenient and effective means of regulating platinum surface stress is conducive to the development of efficient platinum-based catalysts.…”

Section: Introductionmentioning

confidence: 99%

Symmetry‐Induced Regulation of Pt Strain Derived from Pt₃Ga Intermetallic for Boosting Oxygen Reduction Reaction

Gui,

Cheng,

Wang

et al. 2023

Advanced Materials

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Pt‐based fuel cell catalysts with excellent activity and stability for proton‐exchange membrane fuel cells (PEMFCs) have been developed through strain regulation in recent years. Herein, this work demonstrates that symmetry‐induced strain regulation of Pt surface of PtGa intermetallic compounds can greatly enhance the catalytic performance of the oxygen reduction reaction (ORR). With the strain environment varies derived from the lattice mismatch of analogous PtGa core but different symmetry, the Pt surface of the PtGa alloy and the Pt3Ga (Pmm) precisely realize 0.58% and 2.7% compressive strain compared to the Pt3Ga (P4/mmm). Experimental and theoretical results reveal that when the compressive stress of the Pt lattice increases, the desorption process of O* intermediates becomes accelerated, which is conducive to oxygen reduction. The Pt3Ga (Pmm) with high symmetry and compressive Pt surface exhibit the highest mass and specific activities of 2.18 A mgPt−1 and 5.36 mA cm−2, respectively, which are more than one order of magnitude higher than those of commercial Pt/C catalysts. This work demonstrates that material symmetry can be used to precisely modulate Pt surface stress to enhance the ORR, as well as provide a distinct platform to investigate the relationship between Pt compressibility and catalytic activity.

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Enhanced electrocatalytic performance of polyethyleneimine-modified CNTs composite cathode for H2O2 electrogeneration

Xin,

Li,

Huang

et al. 2024

Appl. Phys. A

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Understanding catalytic activity trends of atomic pairs in single-atom catalysts towards oxygen reduction reactions

Cited by 4 publications

References 50 publications

Orbital Orientation-based Theoretical Design of Single-Atom Catalysts for the Hydrogen Evolution Reaction

Orbital Orientation-based Theoretical Design of Single-Atom Catalysts for the Hydrogen Evolution Reaction

Symmetry‐Induced Regulation of Pt Strain Derived from Pt₃Ga Intermetallic for Boosting Oxygen Reduction Reaction

Enhanced electrocatalytic performance of polyethyleneimine-modified CNTs composite cathode for H2O2 electrogeneration

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Understanding catalytic activity trends of atomic pairs in single-atom catalysts towards oxygen reduction reactions

Cited by 4 publications

References 50 publications

Orbital Orientation-based Theoretical Design of Single-Atom Catalysts for the Hydrogen Evolution Reaction

Orbital Orientation-based Theoretical Design of Single-Atom Catalysts for the Hydrogen Evolution Reaction

Symmetry‐Induced Regulation of Pt Strain Derived from Pt3Ga Intermetallic for Boosting Oxygen Reduction Reaction

Enhanced electrocatalytic performance of polyethyleneimine-modified CNTs composite cathode for H2O2 electrogeneration

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Symmetry‐Induced Regulation of Pt Strain Derived from Pt₃Ga Intermetallic for Boosting Oxygen Reduction Reaction