Synthesis of a MoSx–O–PtOx Electrocatalyst with High Hydrogen Evolution Activity Using a Sacrificial Counter‐Electrode

Zhan, Yingxin; Li, Yi; Yang, Zhi; Wu, Xiongwei; Ge, Mengzhan; Zhou, Xuemei; Hou, Junjie; Zheng, Xiannuo; Lai, Yuchong; Pang, Rongrong; Duan, Huan; Chen, Xi’an; Nie, Huagui; Huang, Shaoming

doi:10.1002/advs.201801663

Cited by 21 publications

(13 citation statements)

References 38 publications

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“…The far lower Tafel slope of Pt-SL/TiO 2 also indicates that the Pt valence bonds in the Pt-SL could provide continuous and abundant Pt active sites to absorb and dissociate water, accelerate the sluggish HER in alkaline. [40] This result is also confirmed by the simulated electrocatalytic dynamics (vide infra). The electrochemical stability of Pt-SL/TiO 2 was investigated using the accelerated durability test (ADT) in 1 m KOH solution from 0.6 to 1.0 V (reversible hydrogen electrode, RHE).…”

Section: Performance Evaluation Of Single-layer Pt/tiosupporting

confidence: 61%

Atomic Structural Evolution of Single‐Layer Pt Clusters as Efficient Electrocatalysts

Zhang

Ren

et al. 2021

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Noble metal catalysts, especially Pt, have been widely used for electrochemical energy conversion, including in fuel cells, [1,2] water electrolysis, [3,4] metal-air batteries, [5] and N 2 /CO 2 to fuel conversion. [6][7][8] However, because of the scarcity of Pt, increasing its usage efficient is a significant way to reduce the cost of production. [9][10][11] An efficient strategy is to downsize catalysts, which has been regarded as one of the most effective The rational synthesis of single-layer noble metal directly anchored on support materials is an elusive target to accomplish for a long time. This paper reports well-defined single-layer Pt (Pt-SL) clusters anchored on ultrathin TiO 2 nanosheets-as a new frontier in electrocatalysis. The structural evolution of Pt-SL/TiO 2 via self-assembly of single Pt atoms (Pt-SA) is systematically recorded. Significantly, the Pt atoms of Pt-SL/TiO 2 possess a unique electronic configuration with PtPt covalent bonds surrounded by abundant unpaired electrons. This Pt-SL/TiO 2 catalyst presents enhanced electrochemical performance toward diverse electrocatalytic reactions (such as the hydrogen evolution reaction and the oxygen reduction reaction) compared with Pt-SA, multilayer Pt nanoclusters, and Pt nanoparticles, suggesting an efficient new type of catalyst that can be achieved by constructing single-layer atomic clusters on supports.

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Section: Performance Evaluation Of Single-layer Pt/tiosupporting

confidence: 61%

Atomic Structural Evolution of Single‐Layer Pt Clusters as Efficient Electrocatalysts

Zhang

Ren

et al. 2021

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“…[ 4a,b,24,34 ] The lower Tafel slope of Pt‐SA/ML‐WO 3 (≈27 mV dec −1 ) demonstrates that its inherent HER kinetics is determined by the Volmer‐Tafel reactions, similar to the case of 20 wt% Pt/C, while the higher Tafel slopes of ML‐WO 3 ·H 2 O and ML‐WO 3 (≈98 and 60 mV dec −1 , respectively) suggest that the Volmer–Heyrovsky reaction determines their inherent HER kinetics. [ 10,37 ] The difference in the rate‐determining steps between Pt‐SA/ML‐WO 3 and ML‐WO 3 mainly arises from their different active sites (Pt for Pt‐SA/ML‐WO 3 and W for ML‐WO 3 ).…”

Section: Resultsmentioning

confidence: 99%

“…Many materials have been used as the support for SACs, mainly including metals, [ 8 ] metal oxides, [ 4a,c,9 ] metal carbides [ 3 ] and nitrides (MXenes), [ 4b ] metal sulfides, [ 10 ] and heteroatom‐doped carbon materials. [ 11 ] Recently, tungsten trioxide (WO 3 ), an important member of transition‐metal oxides (TMOs), [ 12 ] as a support has attracted great attention because of its environmental friendliness, earth abundance, and chemical stability, especially its excellent stability in strongly acidic media.…”

Section: Introductionmentioning

confidence: 99%

Single Platinum Atoms Immobilized on Monolayer Tungsten Trioxide Nanosheets as an Efficient Electrocatalyst for Hydrogen Evolution Reaction

Wang

et al. 2021

Adv Funct Materials

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Monolayer WO3·H2O (ML‐WO3·H2O) nanosheets are synthesized via a space‐confined strategy, and then a single‐atom catalyst (SAC) is constructed by individually immobilizing Pt single atoms (Pt‐SA) on monolayer WO3 (ML‐WO3). The Pt‐SA/ML‐WO3 retains the monolayer structure of ML‐WO3·H2O, with a quite high monolayer ratio up to ≈93%, and possesses rich defects (O and W vacancies). It exhibits excellent electrocatalytic performance, with a small overpotential (η) of −22 mV to drive −10 mA cm−2 current, a low Tafel slope of ≈27 mV dec−1, an ultrahigh turnover frequency of ≈87 H2 s−1 site−1 at η = −50 mV, and long‐term stability. Of particular note, it exhibits an ultrahigh mass activity of ≈87 A mgPt−1 at η = −50 mV, which is ≈160 times greater than that of the state‐of‐the‐art commercial catalyst, 20 wt% Pt/C (≈0.54 A mgPt−1). Experimental and DFT analyses reveal that its excellent performance arises from the strong synergetic effect between the single Pt atoms and the support. This work provides an effective route for large‐scale fabrication of ML‐WO3 nanosheets, demonstrates ML‐WO3 is an excellent support for SACs, and also reveals the great potential of SACs in reducing the amount of noble metals used in catalysts.

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“…Compared with wet chemical method, electrochemical deposition (sacrificial-anode Pt sheet) method has been proved to have the advantages of high efficiency, control, and maximum Pt utilization. [5,[46][47][48] Consequently, we applied the CV method for the synthesis of MAC tailored low dose Pt catalyst in 0.5 m H 2 SO 4 system with a Pt foil as the counter electrode. As a matter of course, MAC 1 V 4 h was selected for subsequent experiments due to its lowest HER overpotential.…”

Section: Catalyst Synthesis and Characterization Of Mac@ptmentioning

confidence: 99%

In Situ Electrosynthesis of MAX‐Derived Electrocatalysts for Superior Hydrogen Evolution Reaction

Sheng

Bin

Yang

et al. 2022

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more mature precious metal catalysts such as Pt. However, the high cost, limited earth reserves, and easy aggregation property promote the optimization of precious metal usage and the development of non-precious metal catalysts. [4] Therefore, the coupling mechanism of the conductive matrix and the Pt nanoparticles can greatly stabilize the catalytic activity and reduce the production cost at the same time. [5] 2D transition metal carbides and nitrides (MXenes) of high electrical conductivity, hydrophilicity, large specific surface area, and adjustable surface characteristics have shown great potential in the field of electrocatalysis. [6] MXenes specifically refer to a type of material with M n + 1 X n T x element composition (M, transition metal element, X, C, or N atom, and T, surface functional group, and n = 1-4, atomic layer number). [7] Recently, Cui et al. proposed a method to take advantage of the hydrophilicity and reducibility of MXenes to immobilize highly active nano/atomic metal Pt on Ti 3 C 2 T x MXene sheets, while adding single-walled carbon nanotubes as a binder. The prepared hierarchical HER catalyst (in the form of a membrane) showed high stability during 800 h operation. [8] And a strategy for electrochemical in situ synthesis of Mo 2 TiC 2 T x MXenes supported single platinum atoms was proposed. The vacancy introduced by electrochemical exfoliation of MXenes became the active site anchored by Pt, enhancing the activity of HER. [9] Besides, low Pt dose supported on multilevel hollow MXenes catalyst, Pt 3 Ti nanoparticles formed in situ based on Ti from the surface of Ti 3 C 2 T x , and PtNi ultrathin nanowires with MXenes provided an actual MXenes coupling concept with Pt, enabling the development of high performance and stability of HER catalysts. [4,10,11] According to current literature reports, various surface groups and intrinsic defects of MXene have remarkable effects on the anchoring and dispersion of Pt atoms/cluster. [12] At present, the most extensive preparation method is to etch the A layer atoms in the MAX phase (A represents the elements of 13 or 14 groups in periodic table) by HF or LiF + HCl. Theoretical predictions have confirmed some pure MXenes are promising HER catalysts based on the premise that surface functional groups are O or OH groups. [13] Nevertheless, the experimental results showed poor catalytic activity of pure MXenes, generally due to the wet chemical etching of the precursor MAX phase to prepare MXenes, which introduced MAX phases are frequently dominated as precursors for the preparation of the star material MXene, but less eye-dazzling by their own potential applications. In this work, the electrocatalytic hydrogen evolution reaction (HER) activity of MAX phase is investigated. The MAX-derived electrocatalysts are prepared by a two-step in situ electrosynthesis process, an electrochemical etching step followed by an electrochemical deposition step. First, a Mo 2 TiAlC 2 MAX phase is electrochemically etched in 0.5 m H 2 SO 4 electrolyte. Just several hours...

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Synthesis of a MoS_x–O–PtO_x Electrocatalyst with High Hydrogen Evolution Activity Using a Sacrificial Counter‐Electrode

Cited by 21 publications

References 38 publications

Atomic Structural Evolution of Single‐Layer Pt Clusters as Efficient Electrocatalysts

Atomic Structural Evolution of Single‐Layer Pt Clusters as Efficient Electrocatalysts

Single Platinum Atoms Immobilized on Monolayer Tungsten Trioxide Nanosheets as an Efficient Electrocatalyst for Hydrogen Evolution Reaction

In Situ Electrosynthesis of MAX‐Derived Electrocatalysts for Superior Hydrogen Evolution Reaction

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