Highly Selective Pd Nanosheet Aerogel Catalyst with Hybrid Strain Induced by Laser Irradiation and P Doping Postprocess

Abstract

Strain engineering of electrocatalysts provides an effective strategy to improve the intrinsic catalytic activity. Here, the defect‐rich crystalline/amorphous Pd nanosheet aerogel with hybrid microstrain and lattice strain is synthesized by combining laser irradiation and phosphorus doping methods. The surface strain exhibited by the microstrain and lattice strain shifts the d‐band center of the electrocatalyst, enhancing the adsorption of intermediates in the ethanol oxidation reaction and thus improving the catalytic performances. The measured mass activity, specific activity and C1‐path selectivity of the Pd nanosheet aerogel are 4.48, 3.06, and 5.06 times higher than those of commercial Pd/C, respectively. These findings afford a new strategy for the preparation of highl activity and C1 pathway selective catalysts and provide insight into the catalytic mechanism of strain‐rich heterojunction materials based on tunable surface strain values.

Recent Progress of Amorphous Nanomaterials

“…Jiang’s group prepared defect-rich crystalline/amorphous composite heterojunction Pd nanosheet aerogels with microstrain and lattice strain by laser irradiation and P doping. In this work, CO was injected into a methanol solution containing a surfactant and Pd precursors, and defect-rich Pd nanosheet gels were obtained under continuous laser irradiation (Figure e–g) . Furthermore, Jiao and co-workers synthesized crystalline NiO-amorphous CrO x mixed oxides by a simple hydrothermal method and oxidation treatment (Figure h–o) .…”

“…The fabrication of complex heterogeneous nanosheets by onestep electrostatic deposition is shown in Figure 41d−i. 248 As was mentioned earlier, the amorphous support can contribute to faster electron transfer compared with the 250 Furthermore, Jiao and co-workers synthesized crystalline NiO-amorphous CrO x mixed oxides by a simple hydrothermal method and oxidation treatment (Figure 42h− o). 251 Due to the similar thermal deposition temperature of the precursor, the crystalline-amorphous heterogeneous phase was eventually generated, and the generation of the heterogeneous structure greatly improved the catalytic performance of the material.…”

Recent Progress of Transition Metal Selenides for Electrochemical Oxygen Reduction to Hydrogen Peroxide: From Catalyst Design to Electrolyzers Application

“…Amorphous materials' disordered atomic organization has the potential to greatly increase the efficiency of many electrocatalytic processes. [82][83][84] In order to further improve the catalytic activity and selectivity of palladium selenide, Huang et al [65] prepared amorphous PdSe 2 nanoparticles (a-PdSe 2 NPs) with low coordination Pd sites for the generation of H 2 O 2 . The Pd and Se K-edge XANES profiles confirm that compared to c-PdSe 2 , Pd in a-PdSe NPs/C subject to a substantially lessening of Se's ability to extract electrons (Figure 3a,b).…”

p–d Orbital Hybridization-Engineered PdSn Nanozymes for a Sensitive Immunoassay

“…Recently, the p–d orbital hybridization strategy has been considered an effective way to optimize the electronic structure of catalysts and thus adjust the binding strength of a substrate, which has been extensively investigated in the field of electrocatalysis. − However, the nanozymes involved biomimetic catalysis based on p–d orbital hybridization has rarely been reported. Introducing d-block transition metal doped with p-block metal atoms can introduce additional electronic states or modify the band structure, thereby adjusting the d-band center position. − This adjustment has the potential to alter the interaction between the nanozymes and substrate or reaction intermediate, leading to enhanced catalytic activity and selectivity. − The extraordinary p–d orbital hybridization presents a significant opportunity for the development of nanozymes that achieve high activity and specificity.…”