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laser fragmentation in liquid synthesis of novel palladium-sulfur compound nanoparticles as efficient electrocatalysts for hydrogen evolution reaction

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Chinese Physics B 2022年第7期31卷 34-40页

作者： Guo-Shuai Fu Hong-Zhi Gao Guo-Wei Yang Peng Yu Pu Liu State Key Laboratory of Optoelectronic Materials and Technologies Nanotechnology Research CenterSchool of Materials Science&EngineeringSun Yat-sen UniversityGuangzhou 510275China

One promising way to tune the physicochemical properties of materials and optimize their performance in various potential applications is to engineer material structures at the atomic *** is well known,the performance of Pd-based catalysts has long been constrained by surface contamination and their single ***,we employed an unadulterated top-down synthesis method,known as laser fragmentation in liquid(LFL),to modify pristine Pd PS crystals and obtained a kind of metastable palladium-sulfur compound nanoparticles(LFL-Pd S NPs)as a highly efficient electrocatalyst for hydrogen evolution reaction(HER).laser fragmentation of the layered Pd PS crystal led to a structural reorganization at the atomic level and resulted in the formation of uniform metastable LFL-Pd S ***,the LFL-Pd S NPs show excellent electrocatalytic HER performance and stability in acidic media,with an overpotential of-66 m V at 10 m A·cm^(-2),the Tafel slope of 42 m V·dec^(-1).The combined catalytic performances of our LFL-Pd S NPs are comparable to the Pt/C catalyst for *** work provides a top-down synthesis strategy as a promising approach to design highly active metastable metal composite electrocatalysts for sustainable energy applications.

关键词： Pd-based electrocatalyst hydrogen evolution reaction laser fragmentation in liquid nanoparticles

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Computational study of laser fragmentation in liquid:Phase explosion,inverse Leidenfrost effect at the nanoscale,and evaporation in a nanobubble

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Science China(Physics,Mechanics & Astronomy) 2022年第7期65卷 99-114页

作者： Hao Huang Leonid V.Zhigilei School of Mechanical Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China Department of Materials Science and Engineering University of VirginiaCharlottesville 22904-4745USA

laser fragmentation in liquid is an effective and environment-friendly processing technique capable of yielding colloidal nanoparticles and atomic clusters with a narrow size distribution. The advancement of this technique can be facilitated by an improved understanding of processes that control the sizes, shapes, and structures of the produced nanoparticles. In this work, the dependence of the fragmentation mechanisms on the energy density deposited by the laser pulse is investigated in atomistic simulations performed for 20 nm Au nanoparticles irradiated in water by 10 ps laser pulses. The simulations reveal that the decrease in the absorbed laser energy leads to sequential transitions from the regime of “strong” phase explosion, when all products of an explosive phase decomposition of the irradiated nanoparticle are promptly injected into the water surrounding a nanobubble formed around the nanoparticle, to two distinct regimes of nanoparticle fragmentation leading to the formation of a large central nanoparticle surrounded by smaller satellite fragments. First, in the regime of “mild” phase explosion, the central nanoparticle is produced by the reflection of some of the hot metal droplets generated by the explosive decomposition of the nanoparticle from the boundary of the nanobubble. This reflection is attributed to the inverse Leidenfrost effect acting at the nanoscale. The reflected droplets converge in the center of the nanobubble and coalesce into a single droplet that solidifies shortly after the collapse of the nanobubble. Further decrease in the absorbed laser energy brings the irradiation conditions below the threshold for the phase explosion and results in the formation of a core-satellite structure of the fragmentation products through an interplay of the intense evaporation from the surface of the irradiated nanoparticle, evolution of the nanobubble, and condensation of the metal vapor into clusters and small satellite nanoparticles. The computationa

关键词： laser fragmentation in liquid molecular dynamics simulations phase explosion inverse Leidenfrost effect nanobubble nanoparticles

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