Polymer-Brush-Templated Three-Dimensional Molybdenum Sulfide Catalyst for Hydrogen Evolution

Abstract

Earth-abundant hydrogen evolution catalysts are essential for high-efficiency solar-driven water splitting. Although a significant amount of studies have been dedicated to the development of new catalytic materials, the microscopic assembly of these materials has not been widely investigated. Here, we describe an approach to control the three-dimensional (3D) assembly of amorphous molybdenum sulfide using polymer brushes as a template. To this end, poly(dimethylaminoethyl methacrylate) brushes were grown from highly oriented pyrolytic graphite. These cationic polymer films bind anionic MoS through an anion-exchange reaction. In a final oxidation step, the polymer-bound MoS is converted into the amorphous MoS catalyst. The flexibility of the assembly design allowed systematic optimization of the 3D catalyst. The best system exhibited turnover frequencies up to 1.3 and 4.9 s at overpotentials of 200 and 250 mV, respectively. This turnover frequency stands out among various molybdenum sulfide catalysts. The work demonstrates a novel strategy to control the assembly of hydrogen evolution reaction catalysts.

CuS Nanosheets Decorated with CoS2 Nanoparticles as an Efficient Electrocatalyst for Enhanced Hydrogen Evolution at All pH Values

“…As shown in Figure e, Co 2p peaks appeared at 780.58 and 798.08 eV, along with two small satellite peaks at 786.39 and 802.93 eV, which are assigned to Co 2p 3/2 and Co 2p 1/2 , respectively . The S 2p spectrum (Figure f) exhibited two peaks at 162.28 and 163.46 eV, which well match with S 2– 2p 3/2 and S 2– 2p 1/2 , respectively. , Additionally, the XPS spectra of pure CuS and CoS 2 are shown in Figure S3 (Supporting Information). Figure S3a,b shows the high-resolution XPS spectra of Cu 2p (peaks at 932.13 eV (Cu 2p 3/2 ) and 951.83 eV (Cu 2p 1/2 )) and S 2p (peaks at 162.17 eV (S 2p 3/2 ) and 163.43 eV (S 2p 1/2 )) for the pure CuS.…”

Functionalization of polymers and nanomaterials for water treatment, food packaging, textile and biomedical applications: a review

“…For example, chemically attracted metal nanoparticles to polymer chains, homogenous distribution of functionalized nanoparticles in microgel assembly, polymeric membrane surfaces, or polymer-functionalized metallic thin films (Boyaciyan and von Klitzing 2019). Functionalized polymer brushes for hydrogen evolution were prepared by Stern et al (2018). The highly oriented planar pyrolytic graphite was used for the growth of cationic polyelectrolyte brushes, which catalyze hydrogen production from water by binding molybdenum sulfide of cationic polyelectrolyte.…”

An efficient O-phthalaldehyde-amine coupling reaction for the synthesis of a bottlebrush polymer under physiological conditions

“…[1][2][3] Because of the steric hindrance of the side chains, the backbone is highly extended and exhibits a cylindrical conformation, endowing the bottlebrush polymers with unique structural and physical properties. [4][5][6][7] In the past decade, bottlebrush polymers have demonstrated many potential applications such as drug delivery, 8-10 catalysis, 11,12 antifouling materials, 13,14 lithographic patterning, 15,16 and so on.…”