Trimetallic TriStar Nanostructures: Tuning Electronic and Surface Structures for Enhanced Electrocatalytic Hydrogen Evolution

Du, Nana; Wang, Chengming; Wang, Xijun; Lin, Yue; Jiang, Jun; Xiong, Yujie

doi:10.1002/adma.201504785

Cited by 185 publications

(126 citation statements)

References 46 publications

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“…Platinum, as ‘the Holy Grail’ of HER electrocatalysts, remains the best HER catalysts with nearly zero overpotential and excellent long-term durability3111213. Unfortunately, the widespread commercialization of Pt-based electrocatalysts are hindered by their scarcity and expensive price1415.…”

mentioning

confidence: 99%

Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media

et al. 2017

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The scalable production of hydrogen could conveniently be realized by alkaline water electrolysis. Currently, the major challenge confronting hydrogen evolution reaction (HER) is lacking inexpensive alternatives to platinum-based electrocatalysts. Here we report a high-efficient and stable electrocatalyst composed of ruthenium and cobalt bimetallic nanoalloy encapsulated in nitrogen-doped graphene layers. The catalysts display remarkable performance with low overpotentials of only 28 and 218 mV at 10 and 100 mA cm−2, respectively, and excellent stability of 10,000 cycles. Ruthenium is the cheapest platinum-group metal and its amount in the catalyst is only 3.58 wt.%, showing the catalyst high activity at a very competitive price. Density functional theory calculations reveal that the introduction of ruthenium atoms into cobalt core can improve the efficiency of electron transfer from alloy core to graphene shell, beneficial for enhancing carbon–hydrogen bond, thereby lowing ΔGH* of HER.

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mentioning

confidence: 99%

Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media

et al. 2017

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“…Combined with the polarization curves analyzed above, we may safely draw the conclusion that the 3D porous structure not only contributes to the charge transfer but can also produce an enlarged active area and thus contribute favorably to the final hydrogen evolution. These results also reveal that MoCN-3D is among the most active nonprecious HER electrocatalysts in acidic solutions [6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][32][33][34][35][36][37][38] (Supplementary Tables S3 and S4). …”

Section: Catalytic Performancementioning

confidence: 68%

“…4 In recent years, a wide variety of transition metals (Co, Ni, Fe, Mo and W) and derivative components have been selected as effective candidates. [5][6][7][8][9][10][11] Particularly, β-phase molybdenum carbides have been demonstrated as highly active HER catalysts, even though they are bulky particles, and their performances could be further improved by constructing proper nanostructures. [12][13][14][15][16][17] It was revealed that nanorods of β-Mo 2 C work better as an electrocatalyst for HER than bulk β-Mo 2 C. 12 In addition to the morphology contribution, hybridization with heteroatom-doped graphitic carbon could further improve its performance because the effective coupling between β-Mo 2 C and N-doped graphitic carbon can greatly modify the work function of the hybrid and thus reduce the proton adsorption and the reaction barrier.…”

Section: Introductionmentioning

confidence: 99%

Highly active nonprecious metal hydrogen evolution electrocatalyst: ultrafine molybdenum carbide nanoparticles embedded into a 3D nitrogen-implanted carbon matrix

et al. 2016

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The generation of clean and sustainable hydrogen fuel through water splitting demands efficient and robust earth-abundant catalysts for the hydrogen evolution reaction (HER). A new hybrid, which was fabricated by incorporating molybdenum carbide (Mo x C) nanoparticles into a nitrogen-implanted three-dimensional carbon matrix (MoCN-3D), was developed as a highly active and durable nonprecious metal electrocatalyst for HER. The porous architecture of MoCN-3D can provide continuous mass transportation with a minimal diffusion resistance and thus produce effective electrocatalytic kinetics in both acidic and alkaline media. Experimental observations in combination with density functional theory calculations reveal that the effective coupling between molybdenum carbide nanoparticles and the carbon matrix, as well as N hybrid coordination, can modify the electronic Fermi level of the final hybrid, which synergistically reduces the proton adsorption and the reduction barrier during electrocatalytic HER.

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“…The tunable Tafel slopes observed in our work indicate that the HER occurring at the S sites has been altered by the addition of Pd components [18]. During the process, the bond formation and cleavage of the site-H should have a strong correlation with the electron density of the active sites [19,20]. We thus focus on the interface of Pd with MoS 2 and hypothesize that the difference in work functions (5.12 eV for Pd versus 6.53 eV for MoS 2 ) will induce the accumulation of negative charges on MoS 2 through charge polarization at the Pd-MoS 2 interface [21,22].…”

Section: Resultsmentioning

confidence: 67%

Maneuvering charge polarization and transport in 2H-MoS2 for enhanced electrocatalytic hydrogen evolution reaction

et al. 2016

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Semiconducting 2H-MoS 2 with high chemical stability is a promising alternative to the existing electrocatalysts for the hydrogen evolution reaction (HER); however, the HER performance largely suffers from the limited number of active S sites and low mobility for charge transport. In this work, we demonstrate that the limitations of 2H-MoS 2 for the HER can be overcome by forming hybrid structures with metallic nanowires. Taking the integration with Pd as a proofof-concept, we show with solid experimental evidence that the one-dimensional structure of metallic nanowires facilitates electron transport to active S sites, while the interfacial charge polarization between MoS 2 and Pd increases the electron density of the S sites for improved activity. As a result, the hybrid structure exhibits a current density of 122 mA·cm −2 at −300 mV versus RHE and a Tafel slope of 44 mV·decade −1 with excellent durability, well exceeding the performances of bare 2H-MoS 2 and metallic 1T-MoS 2 . This work provides insights into electrocatalyst design based on charge transport and polarization, which can be extended to other hybrid structures.

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Trimetallic TriStar Nanostructures: Tuning Electronic and Surface Structures for Enhanced Electrocatalytic Hydrogen Evolution

Cited by 185 publications

References 46 publications

Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media

Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media

Highly active nonprecious metal hydrogen evolution electrocatalyst: ultrafine molybdenum carbide nanoparticles embedded into a 3D nitrogen-implanted carbon matrix

Maneuvering charge polarization and transport in 2H-MoS2 for enhanced electrocatalytic hydrogen evolution reaction

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