Regulative Electronic States around Ruthenium/Ruthenium Disulphide Heterointerfaces for Efficient Water Splitting in Acidic Media

Abstract

Theoretical calculations unveil the charge redistribution over abundant interfaces and the enhanced electronic states of Ru/RuS2 heterostructure. The resulting surface electron‐deficient Ru sites display optimized adsorption behavior toward diverse reaction intermediates, thereby reducing the thermodynamic energy barriers. Experimentally, for the first time the laminar Ru/RuS2 heterostructure is rationally engineered by virtue of the synchronous reduction and sulfurization under eutectic salt system. Impressively, it exhibits extremely high catalytic activity for both OER (201 mV @ 10 mA cm−2) and HER (45 mV @ 10 mA cm−2) in acidic media due to favorable kinetics and excellent specific activity, consequently leading to a terrific performance in acidic overall water splitting devices (1.501 V @ 10 mA cm−2). The in‐depth insight into the internal activity origin of interfacial effect could offer precise guidance for the rational establishment of hybrid interfaces.

Anion Modulation of Pt‐Group Metals and Electrocatalysis Applications

“…[11b,13,45] Inspired by this, our group realized the preparation of acidic water splitting electrocatalysts including RuB 2 , RuS 2 , and RuÀ RuS 2 heterostructures by this strategy. [31,46] To obtain the pure-phase RuB 2 with electrocatalytic properties has certain obstacles using other synthesis methods. Thus, we pioneered the introduction of a molten salt system to provide a uniform liquid nucleation environment for the synthesis reaction, thereby successfully synthesizing the pure RuB 2 phase under ordinary pressure.…”

“…[31] Furthermore, for the first time, our group rationally engineered the laminar RuS 2 , and RuÀ RuS 2 with heterostructure interfaces by virtue of the synchronous reduction and sulfurization under an eutectic salt system. [46] Figure 5b exhibit the synthesis schematic and microscopic morphology of RuÀ RuS 2 heterostructures. Due to the electrondeficient Ru sites on the laminar heterostructures, the adsorption behaviors toward OER and HER intermediates were optimized, thereby reducing the thermodynamic energy barriers of water splitting.…”

“…Reproduced with permission. [46] Copyright: 2021, Wiley-VCH. c) Schematic illustration of the synthesis of honeycomb-like microporous IrP 2 @PNPC-NF with abundant step atoms by a new strategy of plasma-assisted calcination.…”

“…[31] Meanwhile, as shown in the Figure 8d and 8e, the Ru/RuS 2 heterostructure first reported by our group also possessed surprising OER performance. [46] Furthermore, Huang's group proposed a precise electrochemical reconstruction strategy of IrTe 2 hollow nanoshuttles (Figure 8f), the selective surface reconstruction of defects helped the Ir-based electrocatalyst show better OER performance than commercial IrO 2 (Figure 8g, h). [53a] Zeng et al prepared a Li-intercalated IrSe 2 electrocatalyst (LiÀ IrSe 2 ) with excellent pH-universal OER activity (Figure 8i).…”

“…Reproduced with permission. [46] Copyright: 2021, Wiley-VCH. f) Schematic illustration of the formation of the defect-rich configuration.…”