Platinum-complexed phosphorous-doped carbon nitride for electrocatalytic hydrogen evolution

Nichols, Forrest; Liu, Qiming; Sandhu, Jasleen; Azhar, Zahra; Cazares, Rafael; Mercado, Rene; Bridges, Frank; Chen, Shaowei

doi:10.1039/d1ta06240a

Title: Platinum-complexed phosphorous-doped carbon nitride for electrocatalytic hydrogen evolution

Journal Article · Tue Sep 21 00:00:00 EDT 2021 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d1ta06240a· OSTI ID:1982222

^[1];

^[1]; Sandhu, Jasleen ^[1]; Azhar, Zahra ^[1]; Cazares, Rafael ^[1]; Mercado, Rene ^[1]; Bridges, Frank ^[1];

^[1]

Univ. of California, Santa Cruz, CA (United States)

Sustainable hydrogen gas production is critical for future fuel infrastructure. Here, a series of phosphorous-doped carbon nitride materials were synthesized by thermal annealing of urea and ammonium hexafluorophosphate, and platinum was atomically dispersed within the structural scaffold by thermal refluxing with Zeise's salt forming Pt–N/P/Cl coordination interactions, as manifested in X-ray photoelectron and absorption spectroscopic measurements. The resulting materials were found to exhibit markedly enhanced electrocatalytic activity towards the hydrogen evolution reaction (HER) in acidic media, as compared to the P-free counterpart. This was accounted for by P doping that led to a significantly improved charge carrier density within C₃N₄, and the sample with the optimal P content showed an overpotential of only –22 mV to reach the current density of 10 mA cm^–2, lower than that of commercial Pt/C (–26 mV), and a mass activity (7.1 mA μg^–1_Pt at –70 mV vs. reversible hydrogen electrode) nearly triple that of the latter. Finally, results from the present study highlight the significance of P doping in the manipulation of the electronic structures of metal/carbon nitride nanocomposites for high-performance HER electrocatalysis.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; CHE-2003685; CHE-1900235; 1126845

OSTI ID:: 1982222

Journal Information:: Journal of Materials Chemistry. A, Vol. 10, Issue 11; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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