A Robust PtNi Nanoframe/N‐Doped Graphene Aerogel Electrocatalyst with Both High Activity and Stability

Abstract

Insufficient catalytic activity and stability and high cost are the barriers for Pt‐based electrocatalysts in wide practical applications. Herein, a hierarchically porous PtNi nanoframe/N‐doped graphene aerogel (PtNiNF‐NGA) electrocatalyst with outstanding performance toward methanol oxidation reaction (MOR) in acid electrolyte has been developed via facile tert‐butanol‐assisted structure reconfiguration. The ensemble of high‐alloying‐degree‐modulated electronic structure and correspondingly the optimum MOR reaction pathway, the structure superiorities of hierarchical porosity, thin edges, Pt‐rich corners, and the anchoring effect of the NGA, endow the PtNiNF‐NGA with both prominent electrocatalytic activity and stability. The mass and specific activity (1647 mA mgPt−1, 3.8 mA cm−2) of the PtNiNF‐NGA are 5.8 and 7.8 times higher than those of commercial Pt/C. It exhibits exceptional stability under a 5‐hour chronoamperometry test and 2200‐cycle cyclic voltammetry scanning.

Tungsten Oxide/Reduced Graphene Oxide Aerogel with Low‐Content Platinum as High‐Performance Electrocatalyst for Hydrogen Evolution Reaction

“…Until now, many efforts have been made on the adequate exposure of all the Pt species in the entire electrode, the activity modulation of each active site, and the stabilization of the active sites during the electrocatalysis. [15] Due to the large surface area, an interconnected 3D network, hierarchical porosity, and the feasibility of structure and composition design of their backbones, aerogels have drawn growing attention, emerged as good candidates for electrocatalysts or their supports, [16][17][18][19][20][21][22][23][24] and shown remarkable electrocatalytic performance in HER. [25] However, the aerogel-based HER electrocatalysts are still limited and mainly restricted to PtAu and AuRh noble-metal backbone aerogels.…”

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

“…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.…”

Interface‐Rich Three‐Dimensional Au‐Doped PtBi Intermetallics as Highly Effective Anode Catalysts for Application in Alkaline Ethylene Glycol Fuel Cells

“…The binding energies (BEs) of Pt 4f 7/2 in Pt 55.1 Bi 44.9 , Pt 51.3 Bi 46.8 Au 1.9 , Pt 53.1 Bi 43.4 Au 3.5 , and Pt 50.9 Bi 43.3 Au 5.8 were found to be 70.56, 70.61, 70.65, and 70.83 eV, respectively, that shifted negatively by 0.84, 0.79, 0.75 and 0.57 eV compared to that of the commercial Pt black (Pt 4f 7/2 : 71.4 eV), showing the existence of strong electronic effects and downshift in the d‐band center of Pt. [ 51–54 ] The valence band spectra (Figure 2d) confirmed that the d‐band center of Pt in the intermetallic Pt 55.1 Bi 44.9 (−3.956 eV) and Pt 53.1 Bi 43.4 Au 3.5 (−3.942 eV) downshifted relative to pure Pt black (−3.774 eV). The downward movement of the d‐band center of Pt weakened the binding strength of the intermediates on the Pt active sites, expedited the reaction kinetics and then dramatically improved the catalytic performances in electrocatalysis.…”