Elucidating the Critical Role of Ruthenium Single Atom Sites in Water Dissociation and Dehydrogenation Behaviors for Robust Hydrazine Oxidation‐Boosted Alkaline Hydrogen Evolution

Li, Jiachen; Li, Yang; Wang, Jiaao; Zhang, Chi; Ma, Huijun; Zhu, Chenhui; Fan, Daidi; Guo, Zhaoqi; Xu, Ming; Wang, Yao‐Yu

doi:10.1002/adfm.202109439

Cited by 97 publications

(75 citation statements)

References 67 publications

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“…As a matter of fact, both HzOR and HER will take place concurrently on the Ni-Co-P/NF catalyst surface in anode chamber (Fig. 6b, path 1), leading to the electroless "spontaneous decomposition" of N 2 H 4 without current (electron) output towards cathode, which is actually not desirable for anode N 2 H 4 oxidation-coupled cathode HER, but widely ignored and indeed inevitable 54 . In order to further study this phenomenon, the gases produced at the cathode and anode were collected by drainage collection method to analyze the actual utilization rates of N 2 H 4 (Fig.…”

Section: Resultsmentioning

confidence: 99%

Active site recovery and N-N bond breakage during hydrazine oxidation boosting the electrochemical hydrogen production

Zhu

Huang

Meng

et al. 2022

Preprint

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Using hydrazine oxidation reaction (HzOR) substituting for oxygen evolution reaction can realize hydrogen production at largely reduced energy consumption. While the HzOR mechanism and the electrochemical utilization rate of hydrazine are still ambiguous. Herein, a bimetallic phosphide heterostructure nanoarrays (Ni-Co-P/NF) fabricated by an interface engineering strategy was used to catalyze both HzOR and hydrogen evolution reaction (HER), and more intensively, probe the HzOR mechanism. The extra-high HzOR performance is attributed to the instantaneous recovery of metal phosphide active site by hydrazine and the extremely low energy barrier with even a new HzOR pathway of N-N bond breakage, which enables the electrolyzer catalyzed by Ni-Co-P/NF to reach 500 mA cm-2 for H2 production at as low as 0.498 V, and offers a high hydrazine electrochemical utilization rate of 93%. The constructed electrolyzer can be powered by the direct hydrazine fuel cell with Ni-Co-P/NF as anodic catalyst, achieving self-powered hydrogen production at the rate up to 19.6 mol h-1 m-2.

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Section: Resultsmentioning

confidence: 99%

Active site recovery and N-N bond breakage during hydrazine oxidation boosting the electrochemical hydrogen production

Zhu

Huang

Meng

et al. 2022

Preprint

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“…Ru-HMT-MP-7║NiFe foam Pyrolysis (ii) 1.50 V@10 mA cm -2 10 h@10 mA cm -2 1.0 m KOH, 25 °C, 1 cm 2 [187] CoNiRu-NT Hydrothermal (i) 1.59 V@50 mA cm -2 48 h@50 mA cm -2 1.0 m KOH, 25 °C, 1.5 cm 2 [176] CC@WS 2 /Ru Galvanostatic deposition (i) 0.31 V@200 mA cm -2 100 h@10 mA cm -2 0.5 m N 2 H 4 + 1.0 m KOH, 25 °C, 3 cm 2 [188] MIL-(IrNiFe)@NF Hydrothermal (i) 0.69V@1000 mA cm -2 12 h@500 mA cm -2 0.5 m N 2 H 4 + 1.0 m KOH + Seawater, 25 °C, 2 cm 2 [189] Ru-Co2P/N-C/NF Pyrolysis (ii) 1.58 V@100 mA cm -2 20 h@1.6 V 0.5 m Urea + 1.0 m KOH, 25 °C, 3 cm 2 [180] CoPt3@Co2P /Co@NCNT Pyrolysis (ii) 1.43 V@10 mA cm -2 12 h@10 mA cm -2 1.0 m CH 3 OH + 1.0 m KOH, 25 °C, 0.5 cm 2 [190] (i), (ii) According to the classification of synthesis strategies in Section 2: (i) directly loading noble metal onto carbon nanomaterials; (ii) carbonizing mixture of noble metal with carbon precursors.…”

Section: Development Of Water Electrolysis Devicesmentioning

confidence: 99%

Recent Advances in Carbon‐Supported Noble‐Metal Electrocatalysts for Hydrogen Evolution Reaction: Syntheses, Structures, and Properties

Liu

Wang

Zhang

et al. 2022

Advanced Energy Materials

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concentration has increased from ≈277 ppm in 1750, prior to Industrial Revolution, to ≈410 ppm in 2019 and the average annual growth of carbon emission in 2018 and 2019 is greater than its 10-year average. [1] Thus, it is urgent to search for renewable and zero-carbon energy sources as alternatives to replace fossil fuels. [2] Although solar, wind and tidal energy are abundant and sustainable, their intermittent and weather-dependent limitations require development and deployment of highly efficient energy conversion and storage systems at large scale to bridge the time gap between supply and demand. [3] An attractive solution is to convert the electrical energy derived from the aforementioned renewable energy sources into chemical energy in the form of hydrogen. [4,5] Pure or mixed hydrogen is playing important roles in transportation, industrial sectors, and chemical transformation processes. [6] However, at present, 95% of hydrogen is still produced by reforming of fossil fuels that emits significant amount of CO 2 and only 4% is through water electrolysis, mainly owing to the much higher production cost of the latter. [7] Therefore, crucial to enable this sustainable vision is to improve the efficiency and scalability of water electrolysis technology.

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“…Moreover, developing high-valueadded products via alternative methods to commercially complex, harmful, and energy-intensive preparation procedures is also desirable. [4,5] For example, some typical co-electrolysis systems, including OWS coupled with more thermodynamically favorable oxidation reactions of urea, [6] hydrazine, [7,8] alcohols, [5] 5-hydroxymethylfurfural, [9] methanol, [10] glycerol, [11] glucose, [12] and sulfion recycling, [13] have been studied extensively.…”

Section: Introductionmentioning

confidence: 99%

Green Electrosynthesis of 5,5′‐Azotetrazolate Energetic Materials Plus Energy‐Efficient Hydrogen Production Using Ruthenium Single‐Atom Catalysts

Zhang

et al. 2022

Advanced Materials

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Water electrolysis involves two parallel reactions, that is, oxygen evolution (OER) and hydrogen evolution (HER), in which sluggish OER is a significant limiting step that results in high energy consumption. Coupling the thermodynamically favorable electrooxidation of organic alternatives to value‐added fine chemicals HER is a promising approach for the simultaneous cost‐effective production of value‐added chemicals and hydrogen. Here, a new coupling system for the green electrochemical synthesis of organic energetic materials (EMs) plus hydrogen production using single‐atom catalysts is introduced. The catalysts are prepared by the facile galvanostatic deposition of ruthenium single atoms on the molybdenum selenide and reveal a low HER overpotential of 38.9 mV at −10 mA cm−2 in an alkaline medium. Importantly, the cell voltage of water electrolysis can be significantly reduced to only 1.35 V at a current of 10 mA cm−2 by coupling water splitting with the electrooxidation of 5‐amino‐1H‐tetrazole to synthesize 5,5′‐azotetrazolate energetic material. These materials are traditionally synthesized under harsh conditions involving a strong oxidizing agent, high‐temperature conditions, and difficult separation of by‐products. This study provides a green and efficient method of synthesizing organic EMs while simultaneously producing hydrogen.

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Elucidating the Critical Role of Ruthenium Single Atom Sites in Water Dissociation and Dehydrogenation Behaviors for Robust Hydrazine Oxidation‐Boosted Alkaline Hydrogen Evolution

Cited by 97 publications

References 67 publications

Active site recovery and N-N bond breakage during hydrazine oxidation boosting the electrochemical hydrogen production

Active site recovery and N-N bond breakage during hydrazine oxidation boosting the electrochemical hydrogen production

Recent Advances in Carbon‐Supported Noble‐Metal Electrocatalysts for Hydrogen Evolution Reaction: Syntheses, Structures, and Properties

Green Electrosynthesis of 5,5′‐Azotetrazolate Energetic Materials Plus Energy‐Efficient Hydrogen Production Using Ruthenium Single‐Atom Catalysts

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