Highly Dispersed Platinum Chlorine Atoms Anchored on Gold Quantum Dots for a Highly Efficient Electrocatalyst

Abstract

The development of efficient and durable electrocatalysts is the only way to achieve commercial fuel cells. A new, efficient method was utilized for epitaxial growth of gold quantum dots using atomically platinum chlorine species with porous graphdiyne as a support (PtCl 2 Au(111)/GDY), for obtaining successful multicomponent quantum dots with a size of 2.37 nm. The electrocatalyst showed a high mass activity of 175.64 A mg Pt −1 for methanol oxidation reactions (MORs) and 165.35 A mg Pt −1 for ethanol oxidation reactions (EORs). The data for this experiment are 85.67 and 246.80 times higher than those of commercial Pt/C, respectively. The catalyst also showed highly robust stability for MORs with negligible specific activity decay after 110 h at 10 mA cm −2 . Both structure characterizations and theoretical calculations reveal that the excellent catalytic performance can be ascribed to the chlorine introduced to modify the d-band structure on the Pt surface and suppression of the CO poisoning pathway of the MOR. Our results indicate that an atomically dispersed metal species tailoring strategy opens up a new path for the efficient design of highly active and stable catalysts.

Rhodium nanocrystals on porous graphdiyne for electrocatalytic hydrogen evolution from saline water

“…Besides, the presence of obvious charge transfer from Rh to GDY make partial Rh species with higher valence states. This result indicates that we obtained the Rh/GDY catalysts with mixed-valence states 25 , 37 , 40 , 45 . The spontaneous recycling of the Rh 0 /Rh + /Rh 3+ , and the specific incomplete charge transfer between multiple valences metal species in this system can endow Rh/GDY with excellent catalytic activity.…”

“…Comprehensive analysis of the current carbon materials, porous graphdiyne (GDY) shows the advantages, 2D layered structure with spand sp 2 -hybridized carbon atoms, large porous structure, infinite distribution of active sites, excellent electron transfer ability, high surface area and high stability . These natural advantages make GDY as a catalyst with excellent comprehensive performance for hydrogen evolution reaction (HER) [30][31][32][33][34][35] , oxygen reduction reaction (ORR) 36,42 , oxygen evolution reaction (OER) 34,35 , overall water splitting (OWS) 34,35 , nitrogen reduction reaction (NRR) 37,38 , CO 2 reduction reaction (CO 2 RR) 39 , methanol oxidation reaction (MOR) 40 and CO catalytic oxidation 41 . In fact, the previous reports have demonstrated GDY to be an ideal catalyst support for selectively anchoring single metal atoms and controllably regulating the coordination environments of metal atoms toward highly catalytic activity.…”

“…In fact, the previous reports have demonstrated GDY to be an ideal catalyst support for selectively anchoring single metal atoms and controllably regulating the coordination environments of metal atoms toward highly catalytic activity. A variety of porous GDY-based catalysts have been developed, e.g., GDY-based zero-valent atomic catalysts [30][31][32] , heterostructured catalysts 34,37 , quantumn dots catalysts 38,[40][41][42] , and metal-free catalysts 35,36 .…”

Graphdiyne Electrochemistry: Progress and Perspectives

“…The mass activity of the MOR was 4.40 A mg Pt+Ni –1 and the specific activity was 136.78 mA cm 2 . [ 193 ] A PtCl 2 Au(111)/GDY that was synthesized using a two‐step method featured extraordinary electrocatalytic MOR and EOR activities. Its mass activities toward the MOR and EOR were 175.64 A mg Pt –1 and 165.35 A mg Pt –1 , respectively.…”

Controlled Growth of the Interface of CdWOx/GDY for Hydrogen Energy Conversion

“…In recent years, the unique and fascinating properties of GDY have brought new knowledge, phenomena, and properties to catalysis, energy conversion and storage, electronics, intelligent devices, and other fields. [ 22–34 ] After years of experimental and theoretical research on GDY, we have accumulated rich experience in fundamental and applied research in the design and construction of the new concept of catalytic and energy conversion devices. It is our responsibility to timely develop such hydrogen energy conversion devices.…”