Room-Temperature Laser Planting of High-Loading Single-Atom Catalysts for High-Efficiency Electrocatalytic Hydrogen Evolution

Abstract

Despite stunning progress in single-atom catalysis (SAC), it remains a grand challenge to yield a high loading of single atoms (SAs) anchored on substrates. Herein, we report a one-step laser-planting strategy to craft SAs of interest under an atmospheric temperature and pressure on various substrates including carbon, metals, and oxides. Laser pulses render concurrent creation of defects on the substrate and decomposition of precursors into monolithic metal SAs, which are immobilized on the as-produced defects via electronic interactions. Laser planting enables a high defect density, leading to a record-high loading of SAs of 41.8 wt %. Our strategy can also synthesize high-entropy SAs (HESAs) with the coexistence of multiple metal SAs, regardless of their distinct characteristics. An integrated experimental and theoretical study reveals that superior catalytic activity can be achieved when the distribution of metal atom content in HESAs resembles the distribution of their catalytic performance in a volcano plot of electrocatalysis. The noble-metal mass activity for a hydrogen evolution reaction within HESAs is 11-fold over that of commercial Pt/C. The laser-planting strategy is robust, opening up a simple and general route to attaining an array of low-cost, high-density SAs on diverse substrates under ambient conditions for electrochemical energy conversion.

Harnessing single-atom catalysts for CO2 electroreduction: a review of recent advances

“…113 (g) Schematic diagram depicting the synthesis of Pt nanoparticles, Pt clusters, and Pt single atoms under laser planting with low, moderate, and high fluences and frequencies, respectively. 118 with the characteristic that Zn-based nitrogen-doped carbon is easily converted into a Zn-N 3 structure at high temperature. 87 The uniformly dispersed Ni-N 3 -C with a metal loading of 0.85 wt.…”

“…4g). 118 The laser pulses created defects on the support and simultaneously decomposed the precursors into metal atoms, which were subsequently immobilized on the as-produced defects via electronic interaction. Using this strategy, a high loading of single atoms of 41.8 wt.% has been achieved.…”

Controllable Synthesis of Solid Catalysts by High-Temperature Pulse

“…In recent years, the deployment of pulsed heating methods has enabled an acceleration of fundamental innovations and technological advances in solid catalyst materials. For example, the ultrafast incorporation of multiple immiscible elements into one crystalline or amorphous nanoparticle, , the kinetically controllable preparation of high-loading sub-3 nm metal nanoparticles, sub-1 nm metal clusters or even single-atom catalysts at low energy and time cost. ,, These representative advances are inextricably linked to the three distinct features of pulsed heating methods, including (i) an extremely high-temperature thermodynamic environment; (ii) an ultrafast kinetic environment; (iii) localized and directed energy delivery. The first provides sufficient energy to drive a chemical reaction for catalyst preparation by increasing the reaction temperatures.…”

Layer Growth Inhibiting Strategy for Superior-Loading Atomic Metal Sites on Ultrathin Layered Double Hydroxides as the Efficient Chemiluminescence Probes

“…However, the laser-planting protocol requires sophisticated instrumentation and skilled personnel. 25 Accordingly, it is critical for the development of facile protocols to highly efficiently anchor massive active atomic centers on nanosupports. 26 Layered double hydroxides (LDHs) are sorts of twodimensional nanosheets consisting of nanoscale layers of metallic hydroxide stacked with alternating anionic layers.…”

“…It is worth noting that Pt SACs with a loading efficiency of 41.8 wt % were obtained on the basis of the formation of high defect density by a laser-planting strategy. However, the laser-planting protocol requires sophisticated instrumentation and skilled personnel . Accordingly, it is critical for the development of facile protocols to highly efficiently anchor massive active atomic centers on nanosupports …”