Atomically Dispersed Ni in Cadmium-zinc Sulfide Quantum Dots for High-performance Visible-light Photocatalytic Hydrogen Production

Overview

Journal Sci Adv

Specialties Biology
Science

Date 2020 Aug 28

PMID 32851158

Citations 7

Authors

D W Su

J Ran

Z W Zhuang

C Chen

S Z Qiao

Y D Li

G X Wang

Affiliations

Soon will be listed here.

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 H production activity of 18.87 mmol hour g. 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 H adsorption thermodynamics. This work demonstrates a synergistic regulation of the physicochemical properties of QDs for high-efficiency photocatalytic H production.

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References

Quan Z, Wang Z, Yang P, Lin J, Fang J . Synthesis and characterization of high-quality ZnS, ZnS:Mn2+, and ZnS:Mn2+/ZnS (core/shell) luminescent nanocrystals. Inorg Chem. 2007; 46(4):1354-60. DOI: 10.1021/ic061917n. View

Li L, Salvador P, Rohrer G . Photocatalysts with internal electric fields. Nanoscale. 2013; 6(1):24-42. DOI: 10.1039/c3nr03998f. View

PATTERSON E, Shelden C, Stockton B . Kubelka-Munk optical properties of a barium sulfate white reflectance standard. Appl Opt. 2010; 16(3):729-32. DOI: 10.1364/AO.16.000729. View

Yu S, Fan X, Wang X, Li J, Zhang Q, Xia A . Efficient photocatalytic hydrogen evolution with ligand engineered all-inorganic InP and InP/ZnS colloidal quantum dots. Nat Commun. 2018; 9(1):4009. PMC: 6167351. DOI: 10.1038/s41467-018-06294-y. View

Wang S, Borisevich A, Rashkeev S, Glazoff M, Sohlberg K, Pennycook S . Dopants adsorbed as single atoms prevent degradation of catalysts. Nat Mater. 2004; 3(3):143-6. DOI: 10.1038/nmat1077. View

Kresse , Furthmuller . Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B Condens Matter. 1996; 54(16):11169-11186. DOI: 10.1103/physrevb.54.11169. View

Qiao B, Wang A, Yang X, Allard L, Jiang Z, Cui Y . Single-atom catalysis of CO oxidation using Pt1/FeOx. Nat Chem. 2011; 3(8):634-41. DOI: 10.1038/nchem.1095. View

Liu H, He Q, Jiang H, Lin Y, Zhang Y, Habib M . Electronic Structure Reconfiguration toward Pyrite NiS via Engineered Heteroatom Defect Boosting Overall Water Splitting. ACS Nano. 2017; 11(11):11574-11583. DOI: 10.1021/acsnano.7b06501. View

Ravel B, Newville M . ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT. J Synchrotron Radiat. 2005; 12(Pt 4):537-41. DOI: 10.1107/S0909049505012719. View

10.

Yamaguchi K, Mizuno N . Efficient heterogeneous aerobic oxidation of amines by a supported ruthenium catalyst. Angew Chem Int Ed Engl. 2003; 42(13):1479-83. DOI: 10.1002/anie.200250779. View

11.

Cao A, Liu Z, Chu S, Wu M, Ye Z, Cai Z . A facile one-step method to produce graphene-CdS quantum dot nanocomposites as promising optoelectronic materials. Adv Mater. 2010; 22(1):103-6. DOI: 10.1002/adma.200901920. View

12.

Zhang H, Zhang P, Qiu M, Dong J, Zhang Y, Lou X . Ultrasmall MoO Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution. Adv Mater. 2018; 31(6):e1804883. DOI: 10.1002/adma.201804883. View

13.

Yu J, Low J, Xiao W, Zhou P, Jaroniec M . Enhanced photocatalytic CO₂-reduction activity of anatase TiO₂ by coexposed {001} and {101} facets. J Am Chem Soc. 2014; 136(25):8839-42. DOI: 10.1021/ja5044787. View

14.

Jiao J, Lin R, Liu S, Cheong W, Zhang C, Chen Z . Copper atom-pair catalyst anchored on alloy nanowires for selective and efficient electrochemical reduction of CO. Nat Chem. 2019; 11(3):222-228. DOI: 10.1038/s41557-018-0201-x. View

15.

Pearson , Ahn , Fultz . White lines and d-electron occupancies for the 3d and 4d transition metals. Phys Rev B Condens Matter. 1993; 47(14):8471-8478. DOI: 10.1103/physrevb.47.8471. View

16.

Anisimov VI , Zaanen , Andersen . Band theory and Mott insulators: Hubbard U instead of Stoner I. Phys Rev B Condens Matter. 1991; 44(3):943-954. DOI: 10.1103/physrevb.44.943. View

17.

Denton , Ashcroft . Vegard's law. Phys Rev A. 1991; 43(6):3161-3164. DOI: 10.1103/physreva.43.3161. View

18.

Sun S, Zeng H . Size-controlled synthesis of magnetite nanoparticles. J Am Chem Soc. 2002; 124(28):8204-5. DOI: 10.1021/ja026501x. View

19.

Simon T, Bouchonville N, Berr M, Vaneski A, Adrovic A, Volbers D . Redox shuttle mechanism enhances photocatalytic H2 generation on Ni-decorated CdS nanorods. Nat Mater. 2014; 13(11):1013-8. DOI: 10.1038/nmat4049. View

20.

Thomson J, Nagashima K, Macdonald P, Ozin G . From sulfur-amine solutions to metal sulfide nanocrystals: peering into the oleylamine-sulfur black box. J Am Chem Soc. 2011; 133(13):5036-41. DOI: 10.1021/ja1109997. View