Promoting Subordinate, Efficient Ruthenium Sites with Interstitial Silicon for Pt‐Like Electrocatalytic Activity

Chen, Hui; Ai, Xuan; Liu, Wang; Xie, Zhoubing; Feng, Wenjiang; Chen, Wei; Zou, Xiaoxin

doi:10.1002/anie.201906394

Cited by 139 publications

(105 citation statements)

References 26 publications

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“…For HER, generally, a moderate hydrogen adsorption Gibbs free energy (∆ G H ≈ 0) is preferred to ensure fast hydrogen adsorption and desorption. [ 3,4,9,33 ] The Δ G H values for different catalysts and corresponding adsorption models are showed in Figure 5 a and Figure S17 (Supporting Information). Compared to Pt, pure Ru surface exhibits a much higher Δ G H (−0.02 eV for Pt(111) and −0.28 eV for Ru(001)).…”

Section: Resultsmentioning

confidence: 99%

Ruthenium Triazine Composite: A Good Match for Increasing Hydrogen Evolution Activity through Contact Electrification

Pei

et al. 2020

Advanced Energy Materials

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The development of Pt‐free catalysts for the alkaline hydrogen evolution reaction (HER), which is widely used in industrial scale water‐alkali electrolyzers, remains a contemporary and pressing challenge. Ruthenium (Ru) has excellent water‐dissociation abilities and could be an alternative water splitting catalyst. However, its large hydrogen binding energy limits HER activity. Here, a new approach is proposed to boost the HER activity of Ru through uniform loading of Ru nanoparticles on triazine‐ring (C3N3)‐doped carbon (triNC). The composite (Ru/triNC) exhibits outstanding HER activity with an ultralow overpotential of ≈2 mV at 10 mA cm−2; thereby making it the best performing electrocatalyst hitherto reported for alkaline HER. The calculated metal mass activity of Ru/triNC is >10 and 15 times higher than that of Pt/C and Pt/triNC. Both theoretical and experimental studies reveal that the triazine‐ring is a good match for Ru to weaken the hydrogen binding on Ru through interfacial charge transfer via increased contact electrification. Therefore, Ru/triNC can provide the optimal hydrogen adsorption free energy (approaching zero), while maintaining the strong water‐dissociation activity. This study provides a new avenue for designing highly efficient and stable electrocatalysts for water splitting.

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Section: Resultsmentioning

confidence: 99%

Ruthenium Triazine Composite: A Good Match for Increasing Hydrogen Evolution Activity through Contact Electrification

Pei

et al. 2020

Advanced Energy Materials

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“…A Tafel slope of ≈30 mV dec −1 indicates the Volmer-Tafel mechanism, where the recombination of two adsorbed H* at two adjacent active sites (i.e., the Tafel step: H* + H* → H 2 ) is the rate-determining step. [35] Higher Tafel slopes of ≈120 and ≈40 mV dec −1 indicate that the Volmer step (the formation of adsorbed H*) and the Heyrovsky step (the combination of an adsorbed H* with a proton in electrolyte), respectively, are the rate-determining steps. [36] In addition, comparative transition-state calculations of the activation energies of the different steps can offer a deeper understanding of the reaction pathway(s) leading to HER.…”

Section: Reaction Mechanism At Her Active Sitesmentioning

confidence: 99%

Active Site Engineering in Porous Electrocatalysts

et al. 2020

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between electrical and chemical energy to store off-peak electricity produced from these resources. The opportunities relate to the fact that electrocatalytic reactions can be employed to convert these excess and off-peak electricity into chemical bonds in molecules. A fascinating prospect is the utilization of renewable electricity for the conversion of abundant resources such as H 2 O, N 2 , and CO 2 into synthetic fuels such as hydrogen, ammonia, hydrocarbons, and alcohols under ambient conditions (Figure 1). Through the reverse processes, clean electricity can be generated from the products, for example, via hydrogen-, ammonia-, or alcohol-powered fuel cells, ultimately resulting in a closed water cycle, nitrogen cycle, or carbon cycle. Hydrogen production via electrocatalytic water splitting, which may enable the hydrogen economy, is a notable example to these. [2] At present, the annual hydrogen production worldwide exceeds more than 65 million tons, mainly for industrial uses such as petroleum refining and ammonia synthesis. Unfortunately, most of the hydrogen is produced from fossil fuels through steam methane reforming and coal gasification and is accompanied by large emission of the greenhouse gas CO 2. Producing hydrogen from water using renewable electricity provides a green and sustainable pathway for future hydrogen energy cycle. In a similar vein, renewable energy-powered electrocatalysis of CO 2 and N 2 reduction produces high-value fuels or fine chemicals such as formic acid (HCOOH), carbon monoxide (CO), methanol (CH 3 OH), and ammonia (NH 3) under ambient conditions. [3] The use of these renewable fuels (e.g., hydrogen and alcohols), instead of petroleum-based fuels, for transportation applications is receiving unprecedented attention because the former are more environmentally friendly and sustainable. Fuel cell technologies based on these fuels can reliably supply electrical energy and are, thus, highly desired for running emerging electric vehicles. [4] To realize the water cycle, carbon cycle, and nitrogen cycle described above, the central reactions are the hydrogen evolution reaction (HER), the CO 2 reduction reaction (CO 2 RR), and the nitrogen reduction reaction (NRR), as well as the oxygenrelated reactions, including the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR), which are important half reactions in electrolyzers and fuel cells, respectively. In these energy conversion processes, electrocatalysts are indispensable. The desired electrocatalysts should both Electrocatalysis is at the center of many sustainable energy conversion technologies that are being developed to reduce the dependence on fossil fuels. The past decade has witnessed significant progresses in the exploitation of advanced electrocatalysts for diverse electrochemical reactions involved in electrolyzers and fuel cells, such as the hydrogen evolution reaction (HER), the oxygen reduction reaction (ORR), the CO 2 reduction reaction (CO 2 RR), the nitrogen reduction reaction (NRR), and the oxyge...

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“…To this end, it is interesting to produce bifunctional materials by the integration of OER and HER catalysts towards water splitting in various media 3 . To address the challenges, catalyzing HER, OER and overall water splitting have been conducted by extensive catalysts, such as oxides, hydroxides, phosphides, nitrides and chalcogenides [4][5][6][7][8][9][10][11] . Thus, it is urgently needed to design earth-abundant and low-cost non-noble-metal catalysts for industrial applications.…”

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confidence: 99%

Engineering active sites on hierarchical transition bimetal oxides/sulfides heterostructure array enabling robust overall water splitting

et al. 2020

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Rational design of the catalysts is impressive for sustainable energy conversion. However, there is a grand challenge to engineer active sites at the interface. Herein, hierarchical transition bimetal oxides/sulfides heterostructure arrays interacting two-dimensional MoOx/MoS2 nanosheets attached to one-dimensional NiOx/Ni3S2 nanorods were fabricated by oxidation/hydrogenation-induced surface reconfiguration strategy. The NiMoOx/NiMoS heterostructure array exhibits the overpotentials of 38 mV for hydrogen evolution and 186 mV for oxygen evolution at 10 mA cm−2, even surviving at a large current density of 500 mA cm−2 with long-term stability. Due to optimized adsorption energies and accelerated water splitting kinetics by theory calculations, the assembled two-electrode cell delivers the industrially relevant current densities of 500 and 1000 mA cm−2 at record low cell voltages of 1.60 and 1.66 V with excellent durability. This research provides a promising avenue to enhance the electrocatalytic performance of the catalysts by engineering interfacial active sites toward large-scale water splitting.

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Promoting Subordinate, Efficient Ruthenium Sites with Interstitial Silicon for Pt‐Like Electrocatalytic Activity

Cited by 139 publications

References 26 publications

Ruthenium Triazine Composite: A Good Match for Increasing Hydrogen Evolution Activity through Contact Electrification

Ruthenium Triazine Composite: A Good Match for Increasing Hydrogen Evolution Activity through Contact Electrification

Active Site Engineering in Porous Electrocatalysts

Engineering active sites on hierarchical transition bimetal oxides/sulfides heterostructure array enabling robust overall water splitting

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