Engineering Pt Coordination Environment with Atomically Dispersed Transition Metal Sites Toward Superior Hydrogen Evolution

Abstract

Metal single‐atom (SA) catalysts have attracted immense attention due to the high catalytic efficiency given by the desired coordination environment of each metal atom. Yet, engineering the local electronic structure of SAs and multi‐atoms (MAs) still remains a challenge. Herein, an atomically dispersed catalyst comprised of Pt SAs, Pt‐Pt/V dual‐atoms, and small clusters supported on a vanadium and nitrogen co‐doped carbon (VNC) (denoted as Pt@VNC) surface is synthesized. In the Pt@VNC, both V and Pt atoms are evenly distributed on the surface of N‐doped carbon, while a few Pt atoms are linked to other Pt atoms via V, forming Pt clusters. The coordination structures of Pt atoms are modulated upon introducing atomically dispersed V sites (which generate small‐sized Pt clusters) and V2O5 clusters, showing extraordinary activity for the hydrogen evolution reaction (HER). Benefiting from the low charge transfer resistance, i.e., fast reaction kinetics, due to the synergistic effect of SAs and clusters, the Pt@VNC demonstrates superior catalytic efficiency and robust durability for the HER. It requires an overpotential of only 5 mV at a current density of 10 mA cm−2 and shows 15 times larger mass activity than the commercial 20 wt.% Pt/C catalyst. This novel catalyst‐design strategy paves a new way for maximizing catalytic efficiency by optimizing the coordination structure of metal atoms.

Metal-Doped C3B Monolayer as the Promising Electrocatalyst for Hydrogen/Oxygen Evolution Reaction: A Combined Density Functional Theory and Machine Learning Study

“…Meanwhile, the low OER overpotentials are shown for Pt/Ni–N 2 C 2 (0.27/0.40 V), Ni/Pd–C 4 (0.31/0.36 V), and Rh–N 4 (0.31 V) moieties and the Rh-doped borophene (0.24 V) . Ni-doped MXenes are considered as promising candidates for water splitting, with the overall overpotential smaller than 0.48 V. , In an experiment, Jin et al prepared the Pt support on a V/N-codoped carbon, which exhibits excellent HER activity with an overpotential of only 5 mV at a current density of 10 mA cm –2 . Thangavel et al developed a high-efficiency OER electrode via electrochemical integration of amorphous NiFeOOH on carbon fiber paper with an overpotential of η­(O 2 ) only 170 mV.…”

High Entropy Alloy CoCrFeNiMo Reinforced Electrocatalytic Performance for High‐Efficient Electrocatalytic Water Splitting

“…At the same time, it can be seen that the properties of the prepared materials are significantly higher than those of the reported electrocatalysts (Table S1). [42][43][44][45][46][47][48][49][50][51][52][53][54][55][56][57] In addition, the outstanding OER electrocatalytic activity of the CoCrFeNiMo catalyst also can be further demonstrated by its ECSA. Figure 4c shows the C dl value of the CoCrFeNiMo catalyst presents higher electrochemical activity (8.56 mF cm À 2 ) than that of the CoCrFeNi catalyst (4.08 mF cm À 2 ), which also confirms rich electrochemical active sites of the CoCrFeNiMo catalyst.…”

RuO2 Nanostructure as an Efficient and Versatile Catalyst for H2 Photosynthesis

“…H 2 generation, since it is a multielectron process, is boosted by a hydrogen evolution catalyst (HEC), which can be either a molecule or a material. ,− Among the plethora of HECs, the most widely used are platinum and Pt-based catalysts, ,− which are very efficient, but, due to its high cost, low availability, and tendency to be poisoned by several compounds, their implementation remains extremely challenging . Other noble metals demonstrated activity in HER, , and among them, ruthenium, which is at least 6 times cheaper than Pt, has already been employed in 1979, but it gained greater attention only in the last few years, showing HER overpotential at 10 mA cm –2 very close to that of Pt. , Moreover, the oxides of Pt group metals are widely used as an oxygen evolution catalyst (OEC), − but some of them also showed good activity in HER . In particular, ruthenium (IV) oxide (RuO 2 ) has been extensively studied as an OEC, − scarcely for H 2 evolution, and mostly as an electro- ,− or a photoelectro-HEC, − but it is growing as demonstrated by the increasing number of papers since the last 10 years (Figure S1).…”