Atomically dispersed Ni in cadmium-zinc sulfide quantum dots for high-performance visible-light photocatalytic hydrogen production

Abstract

Catalysts with a single atom site allow highly tuning of the activity, stability, and reactivity of heterogeneous catalysts. Therefore, atomistic understanding of the pertinent mechanism is essential to simultaneously boost the intrinsic activity, site density, electron transport, and stability. Here, we report that atomically dispersed nickel (Ni) in zincblende cadmium–zinc sulfide quantum dots (ZCS QDs) delivers an efficient and durable photocatalytic performance for water splitting under sunlight. The finely tuned Ni atoms dispersed in ZCS QDs exhibit an ultrahigh photocatalytic H2 production activity of 18.87 mmol hour−1 g−1. It could be ascribed to the favorable surface engineering to achieve highly active sites of monovalent Ni(I) and the surface heterojunctions to reinforce the carrier separation owing to the suitable energy band structures, built-in electric field, and optimized surface H2 adsorption thermodynamics. This work demonstrates a synergistic regulation of the physicochemical properties of QDs for high-efficiency photocatalytic H2 production.

Atomically Dispersed Catalytic Sites: A New Frontier for Cocatalyst/Photocatalyst Composites toward Sustainable Fuel and Chemical Production

“…As for the co-precipitation method, single atoms are immobilized on the supports during their formation process. This method is suitable for support materials such as g-C 3 N 4 , MOF, metal sulfides, and metal [123][124][125]. For example, Lu et al prepared a series of single-atom Mo catalysts by calcining low-cost primary material of urea with various amounts of Mo(VI) salts [126].…”

Heterostructured MOFs photocatalysts for water splitting to produce hydrogen

“…Moreover, studies have shown that its distribution position in MOFs [54][55][56], dispersion state [20], surface charge state [57] all have important impacts on its charge separation efficiency. In addition, the development of non-precious metal co-catalyst is also a hot spot [58]. For example, transition metal [59] and their phosphides [60] are wrapped in MOFs to achieve high catalytic efficiency.…”

Simultaneous Conduction and Valence Band Regulation of Indium-Based Quantum Dots for Efficient H2 Photogeneration

“…Hence, synthesis of efficient and low-cost photocatalysts is with vital importance for solar-to-fuel conversion. The semiconductor quantum dots (QDs) which the size is less than their exciton Bohr radius in three dimensions have been attracted tremendous attention in this field owing their unique properties, such as large surface area, abundant surface active sites, multiple exciton generation, short charge transfer distance and so on [ 6 , 7 , 8 , 9 , 10 , 11 ]. Among the popular chalcogenide semiconductor-based QDs in artificial photocatalysis, the indium-based chalcogenides seem to be more promising photocatalysts due to their less toxic, noble metal-free as well as the potential visible light harvesting [ 12 , 13 , 14 , 15 ].…”