TY - JOUR
T1 - Photochemical engineering unsaturated Pt islands on supported Pd nanocrystals for a robust pH-universal hydrogen evolution reaction
AU - Liu, Yidan
AU - Yodsin, Nuttapon
AU - Li, Ting
AU - Wu, Haocheng
AU - Jia, Rongrong
AU - Shi, Liyi
AU - Lai, Zhuangchai
AU - Namuangruk, Supawadee
AU - Huang, Lei
N1 - Publisher Copyright:
© 2024 The Royal Society of Chemistry.
PY - 2024/1/30
Y1 - 2024/1/30
N2 - The rational design of heterostructured nanocrystals (HNCs) is of great significance for developing highly efficient hydrogen evolution reaction (HER) electrocatalysts. However, a significant challenge still lies in realizing the controllable synthesis of desired HNCs directly onto a support and exploring their structure-activity-dependent HER performance. Herein, we reported various controllable Pd7@Ptx core-shell HNCs with optimal hybrid structures via a photochemical deposition strategy. The growth patterns of a Pt shell can be finely controlled by adjusting the growth kinetics, resulting in a varying deposition rate. In particular, the as-prepared Pd7@Pt3 HNCs with a Pt shell in the Stranski-Krastanov mode showed the best performances over a wide pH range media, delivering low overpotentials of 33, 18 and 49 mV, resulting in a catalytic current density of 10 mA cm−2 at a low effective catalyst loading of 0.021 mg cm−2. The resulting Tafel slopes were 23.1, 52.6 and 42.7 mV dec−1 in 0.5 M H2SO4, 1.0 M phosphate-buffered saline (PBS) and 1.0 M KOH electrolyte, respectively. It was found that the increased fraction of unsaturated coordination of Pt islands in the resultant material is the key to the enhanced and robust HER activity, which has been confirmed through density functional theory (DFT) calculations. This strategy could be extended to the rational design and synthesis of other heterostructured catalysts for energy conversion and storage.
AB - The rational design of heterostructured nanocrystals (HNCs) is of great significance for developing highly efficient hydrogen evolution reaction (HER) electrocatalysts. However, a significant challenge still lies in realizing the controllable synthesis of desired HNCs directly onto a support and exploring their structure-activity-dependent HER performance. Herein, we reported various controllable Pd7@Ptx core-shell HNCs with optimal hybrid structures via a photochemical deposition strategy. The growth patterns of a Pt shell can be finely controlled by adjusting the growth kinetics, resulting in a varying deposition rate. In particular, the as-prepared Pd7@Pt3 HNCs with a Pt shell in the Stranski-Krastanov mode showed the best performances over a wide pH range media, delivering low overpotentials of 33, 18 and 49 mV, resulting in a catalytic current density of 10 mA cm−2 at a low effective catalyst loading of 0.021 mg cm−2. The resulting Tafel slopes were 23.1, 52.6 and 42.7 mV dec−1 in 0.5 M H2SO4, 1.0 M phosphate-buffered saline (PBS) and 1.0 M KOH electrolyte, respectively. It was found that the increased fraction of unsaturated coordination of Pt islands in the resultant material is the key to the enhanced and robust HER activity, which has been confirmed through density functional theory (DFT) calculations. This strategy could be extended to the rational design and synthesis of other heterostructured catalysts for energy conversion and storage.
UR - http://www.scopus.com/inward/record.url?scp=85185150587&partnerID=8YFLogxK
U2 - 10.1039/d3mh02041j
DO - 10.1039/d3mh02041j
M3 - Journal article
C2 - 38348699
AN - SCOPUS:85185150587
SN - 2051-6347
VL - 11
SP - 1964
EP - 1974
JO - Materials Horizons
JF - Materials Horizons
IS - 8
ER -