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Exceptional Electrochemical HER Performance with Enhanced Angewandte Research Articles Chemie How to cite: Electrocatalysis International Edition: doi.org/10.1002/anie.202103557 German Edition: doi.org/10.1002/ange.202103557 Exceptional Electrochemical HER Performance with Enhanced Electron Transfer between Ru Nanoparticles and Single Atoms Dispersed on a Carbon Substrate Panpan Su+, Wei Pei+, Xiaowei Wang, Yanfu Ma, Qike Jiang, Ji Liang,* Si Zhou,* Jijun Zhao, Jian Liu,* and Gao Qing (Max) Lu Abstract: Precisely regulating the electronic structures of metal their strong electronic metal–support interaction (EMSI),[3] active species is highly desirable for electrocatalysis. However, which enables the modulation of the electronic structure and carbon with inert surface provide weak metal–support inter- catalytic property of metal nanoparticles. On the other hand, action, which is insufficient to modulate the electronic struc- carbon materials as substrates possess superior electrical tures of metal nanoparticles. Herein, we propose a new method conductivity and high chemical stability.[4] However, carbon to control the electrocatalytic behavior of supported metal materials with a relatively inert surface can only provide weak nanoparticles by dispersing single metal atoms on an O-doped EMSI with metal nanoparticles, which is often insufficient to graphene. Ideal atomic metal species are firstly computation- effectively steer the electronic structures of the loaded metal ally screened. We then verify this concept by deposition of Ru nanoparticles. nanoparticles onto an O-doped graphene decorated with single To address this challenge, several strategies have been metal atoms (e.g., Fe, Co, and Ni) for hydrogen evolution proposed for optimizing the EMSI of carbon-based electro- reaction (HER). Consistent with theoretical predictions, such catalysts. For instance, doping carbon substrates with non- hybrid catalysts show outstanding HER performance, much metal elements can induce the redistribution of electrons or superior to other reported electrocatalysts such as the state-of- the spin state of the sp2 conjugated carbon matrix, thus the-art Pt/C. This work offers a new strategy for modulating the tailoring the valence orbital energy of the active sites on activity and stability of metal nanoparticles for electrocatalysis carbon surface.[5] Besides, carbon surface functionalization processes. using oxygen-containing groups can also introduce extra electronic states near the Fermi level, which alters its surface Introduction reactivity.[6] The enhanced EMSI results in strong orbital hybridization between metal nanoparticles and carbon sur- Precise tailoring and controlling of the electronic struc- face, which is beneficial for electron transfer at their interface. ture of a catalyst have long been pursued for achieving Distinct from non-metal dopants or functional groups for outstanding catalytic performance.[1] Conventionally, manip- surface modification, metallic dopants carry more versatile ulation of catalysts surface electronic states can be realized electronic states, which can be more effective for activating by particle size/shape tuning, hetero-element doping, organic the inert carbon surface, thus providing additional opportu- ligands microenvironment engineering, and substrate inter- nities for tailoring the metal particle-support interaction and action.[2] To date, oxide materials have been considered as their associated catalytic characteristics. Indeed, metal single favorable substrates to support metal nanoparticles, due to atoms have been incorporated into carbon frameworks (i.e., [*] Dr. P. Su,[+] Dr. Y. Ma, Prof. J. Liu Prof. J. Liu State Key Laboratory of Catalysis, Dalian Institute of Chemical DICP-Surrey Joint Centre for Future Materials, University of Surrey Physics, Chinese Academy of Sciences Guildford, Surrey, GU2 7XH (UK) 457 Zhongshan Road, Dalian 116023 (China) E-mail: [email protected] E-mail: [email protected] Prof. G. Q. Lu W. Pei,[+] Prof. S. Zhou, Prof. J. Zhao University of Surrey Key Laboratory of Materials Modification by Laser, Ion and Electron Guildford, Surrey, GU2 7XH (UK) Beams (Dalian University of Technology), Ministry of Education [+] These authors contributed equally to this work. Dalian 116024 (China) Supporting information and the ORCID identification number(s) for E-mail: [email protected] the author(s) of this article can be found under: Dr. X. Wang, Prof. J. Liang https://doi.org/10.1002/anie.202103557. Key Laboratory for Advanced Ceramics and Machining Technology of 2021 The Authors. Angewandte Chemie International Edition Ministry of Education, Tianjin University published by Wiley-VCH GmbH. This is an open access article under Tianjin 300350 (China) the terms of the Creative Commons Attribution License, which E-mail: [email protected] permits use, distribution and reproduction in any medium, provided Dr. Q. Jiang the original work is properly cited. Division of Energy Research Resources, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 457 Zhongshan Road, Dalian 116023 (China) &&&& 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH Angew. Chem. Int. Ed. 2021, 60,2–9 Ü Ü These are not the final page numbers! Angewandte Research Articles Chemie single-atom catalysts) to catalyze a serial of electrochemical processes. For example, a variety of metal atoms or their clusters (e.g., Fe, Co, Ni, Cu, Pt, Ru, and Pd) have been coordinated on carbon surface for electrocatalysis of water [7] splitting, nitrogen fixation, and CO2 reduction etc. Besides directly serving as the active sites, these metal centers on the carbon surface, as mentioned above, might have the capability for interacting with secondary metal nanoparticles when they are loaded together on a carbon substrate, which is rarely investigated to the best of our knowledge. Taking Ru nanoparticles on a carbon substrate as a pro- totype system, our density functional theory (DFT) calcula- tions suggest that enhanced charge transfer occurs at the interface between the substrate and Ru nanoparticles, when proper single metal atoms (e.g., Fe, Co, and Ni) are doped in the carbon support. This can effectively reshape the electronic structure of the Ru nanoparticles and enables the optimiza- tion of electrocatalytic activity.[8] To experimentally validate this prediction, Ru nanoparticles, an ideal alternative for the high-cost Pt, were loaded on an O-doped graphene substrate decorated with non-noble-metal single atoms (Fe, Co, or Ni) to serve as model electrocatalysts. Hydrogen evolution Figure 1. a) Atomic structures of Ru55 supported on O-doped graphene reaction (HER), which is hindered by the excessively strong with dispersed metal atoms obtained by DFT calculations. The C, O, binding of H atoms on pristine Ru surface,[9] was chosen as metal, and Ru atoms are shown in gray, red, purple, and turquoise a prototype reaction. This hybrid catalyst comprised of both colors, respectively. b) Bader charge analysis projected to Ru55 cluster. The positive (negative) charge indicates the electron loss (gain) from Ru nanoparticles and dispersed metal atoms exhibits an the Ru atoms. c) Binding energies (Ebind, left axis) of Ru55/M1@OG and ultralow Tafel slope of 22.8 mVdecÀ1 and an extremely low freestanding Ru55, and its corresponding adsorption free energy of H* À2 overpotential of 13 mV at a current density of 10 mAcm , species (DGH*, right axis). d) Density of states (DOS) for Ru55/ which is the highest performance reported by far to the best of M1@OG. The occupied states were shadowed. The dashed line our knowledge. This clearly confirms that Ru nanoparticles indicates the Fermi level for each system. are the active centers and the atomic Co species enhanced HER activity, which is well consistent with the DFT calculation results. Thus, this work offers a universal strategy suggests that these transferred electrons (0.87–0.93e) are for precisely tailoring the electronic structure, activity, and carried by the C atoms nearby the O atoms (electron-rich C stability of metal nanoparticles via a non-destructive and sites in Figure 1a), which would occupy the C pz orbitals and flexible route for various electrocatalytic reactions. break the p conjugation of the graphitic sheet. As a result, the carbon substrate is more reactive to interact with Ru55, gaining more electrons from Ru55 in comparison with Ru55/ Results and Discussion OG (Table 1), and inducing significant charge redistribution on the nanocluster. As illustrated in Figure 1b, for Ru55/ First, this strategy was conceptually investigated by DFT M1@OG, the Ru atoms close to the interfacial region show calculations. As shown in Figure 1a, a highly stable Ru55 a more positive charge density of 0.20–0.22e (compared to cluster with cuboctahedral geometry and a diameter of about 0.13e for Ru55/OG), indicative of a weakened binding 1.2 nm was adopted and supported on an O-doped graphitic strength with H* species and possibly higher activity for nanosheet with highly dispersed transition metal single atoms (denoted as M @OG, with M = Fe, Co, and Ni). The shape and 1 Table 1: Key parameters of Ru nanoclusters supported on various size effects on the activity of metal nanoparticles have been graphene-based substrates.[a] extensively explored[10] and thus will not be considered here. Model e CT CT D [eV] The electronic density of states (DOS) in Figure 1d reveals Ebind d 1 GH* [eV] [eV] (e) (e) that the decoration of single metal atoms introduces prom- inent states near the Fermi level, which activate the inert Ru55 – À2.28 – 0.03 À0.27 carbon surface and remarkably enhance its interaction with Ru55/G 6.98 À2.26 1.41 0.19 À0.23 Ru55/OG 9.88 À2.52 1.58 0.13 À0.11 Ru55. Specifically, the binding strength of Ru55 on Fe1/Co1/ Ru55/Fe1@OG 14.44 À2.59 1.65 0.20 0.02 Ni1@OG substrates becomes over 3.5 eV stronger than that of Ru55/Co1@OG 13.78 À2.55 1.63 0.21 0.05 Ru55 on OG without metal-atom decoration, as demonstrated Ru55/Ni1@OG 13.41 À2.60 1.61 0.22 0.04 in Figure 1c.
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