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Cheong, Soshan

Publications and source records attributed to Cheong, Soshan.

Electronegativity-Guided Site Differentiation in High-Entropy Alloy for pH-universal Hydrogen Evolution Reactions

Enhancing the intrinsic activity of transition metal catalysts for the hydrogen evolution reaction (HER) remains a critical challenge in sustainable energy conversion. Herein, we report an electronegativity-guided site differentiation strategy in a single-phase CoNiCuMoW high-entropy alloy (HEA) via electrodeposition by incorporating high-electronegativity 4d/5d orbital transition metals (Mo, W) into the face-centered cubic (fcc) matrix (CoNiCu). The as-synthesized HEA demonstrates exceptional HER performance in all pH conditions, delivering an outstanding overpotential of 65 mV (alkaline), 28 mV (acidic), and 155 mV (neutral) at a current density of 100 mA cm−2, showing performance comparable to commercial Pt/C and has excellent long-term stability at high current density (1 A cm−2, 1000 h). X-Ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations reveal that the incorporation of Mo/W simultaneously alters the local coordination environment and induces element-dependent charge redistribution, accompanied by a system-level d-band center downshift, thereby optimizing the hydrogen binding strength across multimetallic sites. Meanwhile, oxophilic Mo/W sites lower the water dissociation energy barrier. These synergistic effects collectively enable efficient and durable pH-universal HER performance.

Wu, Yutong↗

Resolving Atomic-Scale Structure and Chemical Coordination in High-Entropy Alloy Electrocatalysts for Structure–Function Relationship Elucidation

The recent breakthrough in confining five or more atomic species in nanocatalysts, referred to as high-entropy alloy nanocatalysts (HEAs), has revealed the possibilities of multielemental interactions that can surpass the limitations of binary and ternary electrocatalysts. The wide range of potential surface configurations in HEAs, however, presents a significant challenge in resolving active structural motifs, preventing the establishment of structure-function relationships for rational catalyst design and optimization. Here, we present a methodology for creating sub-5 nm HEAs using an aqueous-based peptide-directed route. Using a combination of pair distribution function and X-ray absorption spectroscopy, HEA structure models are constructed from reverse Monte Carlo modeling of experimental data sets and showcase a clear peptide-induced influence on atomic-structure and chemical miscibility. Coordination analysis of our structure models facilitated the construction of structure-function correlations applied to electrochemical methanol oxidation reactions, revealing the complex interplay between multiple metals that leads to improved catalytic properties. Our results showcase a viable strategy for elucidating structure-function relationships in HEAs, prospectively providing a pathway for future materials design.

36 MATERIALS SCIENCE↗

A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation

Single Pt atom catalysts are key targets because a high exposure of Pt substantially enhances electrocatalytic activity. In addition, PtRu alloy nanoparticles are the most active catalysts for the methanol oxidation reaction. To combine the exceptional activity of single Pt atom catalysts with an active Ru support we must overcome the synthetic challenge of forming single Pt atoms on noble metal nanoparticles. In this report we demonstrate a process that grows and spreads Pt islands on Ru branched nanoparticles to create single-Pt-atom-on-Ru catalysts. By following the spreading process by in situ TEM, we found that the formation of a stable single atom structure is thermodynamically driven by the formation of strong Pt–Ru bonds and the lowering of the surface energy of the Pt islands. The stability of the single-Pt-atom-on-Ru structure and its resilience to CO poisoning result in a high current density and mass activity for the methanol oxidation reaction over time.

36 MATERIALS SCIENCE↗

Flexible and efficient perovskite quantum dot solar cells via hybrid interfacial architecture

All-inorganic CsPbI 3 perovskite quantum dots have received substantial research interest for photovoltaic applications because of higher efficiency compared to solar cells using other quantum dots materials and the various exciting properties that perovskites have to offer. These quantum dot devices also exhibit good mechanical stability amongst various thin-film photovoltaic technologies. We demonstrate higher mechanical endurance of quantum dot films compared to bulk thin film and highlight the importance of further research on high-performance and flexible optoelectronic devices using nanoscale grains as an advantage. Specifically, we develop a hybrid interfacial architecture consisting of CsPbI 3 quantum dot/PCBM heterojunction, enabling an energy cascade for efficient charge transfer and mechanical adhesion. The champion CsPbI3 quantum dot solar cell has an efficiency of 15.1% (stabilized power output of 14.61%), which is among the highest report to date. Building on this strategy, we further demonstrate a highest efficiency of 12.3% in flexible quantum dot photovoltaics.

14 SOLAR ENERGY↗

Facettierte verzweigte Nickel‐Nanopartikel mit variierbarer Verzweigungslänge für die hochaktive elektrokatalytische Oxidation von Biomasse

Abstract Die Kontrolle der Bildung von verzweigten Nanopartikeln mit hoher Homogenität ist eine der größten Herausforderungen bei der Herstellung von Nanokatalysatoren mit verbesserter Aktivität und Stabilität. Mithilfe eines Mechanismus unter Nutzung eines kubischen Kerns und hexagonaler Verzweigung zur Bildung hochgradig monodisperser verzweigter Nanopartikel wurde die Länge der Nickelverzweigungen variiert. Es hat sich gezeigt, dass die Verlängerung der Nickelzweige mit ihrer hohen Bedeckung der aktiven Facetten die Aktivität für die elektrokatalytische Oxidation von 5‐Hydroxymethylfurfural (HMF) als Beispiel für die Umwandlung von Biomasse verbessert.

Poerwoprajitno, Agus R.↗

Controlling Pt Crystal Defects on the Surface of Ni–Pt Core–Shell Nanoparticles for Active and Stable Electrocatalysts for Oxygen Reduction

A strategy of direct growth of Pt on Ni was used to create and control Pt crystal defects on the surface of Ni–Pt core–shell nanoparticles. The control over the types of defects was easily achieved by changing the surfactant system. Here, in this work, two types of crystal defects have been introduced into Ni–Pt core–shell nanoparticles: polycrystalline shells with multiple grain boundaries and step-edge shells with undercoordinated atoms at corners and steps. We show that the step-edge shell has a higher specific activity for the oxygen reduction reaction (ORR), while the thinner polycrystalline shell results in a higher activity per mass and stability. Our results suggest that Ni–Pt core–shell nanoparticles with a thin Pt shell that have high density of crystal defect should be targeted for high performance ORR catalysts.

36 MATERIALS SCIENCE↗