4.6 Article

Self-driven dual hydrogen production system based on a bifunctional single-atomic Rh catalyst

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 10, Issue 11, Pages 6134-6145

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta07375c

Keywords

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Funding

  1. National Natural Science Foundation of China [22075211, 21601136, 51971157, 12074017, 51621003]
  2. Tianjin Science Fund for Distinguished Young Scholars [19JCJQJC61800]
  3. Beijing Municipal High-Level Innovative Team Building Program [IDHT20190503]
  4. Guangdong Province Higher Vocational Colleges & Schools Pearl River Scholar Funded Scheme
  5. Guangdong Third Generation Semiconductor Engineering Technology Development Center [2020GCZX007]
  6. Science and Technology Development Fund of Tianjin Education Commission for Higher Education [2018KJ126]

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A novel self-driven dual hydrogen production system has been proposed for efficient hydrogen production using highly-dispersed single Rh atoms supported on a catalyst. The system achieves an ultra-high H-2 generation rate and exhibits remarkable catalytic activities towards hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR). Experimental results and density functional theory calculations confirm the excellent catalytic properties of the catalyst.
Electrocatalytic hydrogen evolution is an efficient and economical technology to address environmental contamination and energy crises, but the development of such a high-efficiency and energy-saving sustainable hydrogen production system remains a great challenge. Here, we present a novel strategy to design a self-driven dual hydrogen production system for efficient hydrogen production based on highly-dispersed single Rh atoms supported on an oxygen-functionalized Ti3C2Ox MXene (Rh-SA/Ti3C2Ox) catalyst. The bifunctional Rh-SA/Ti3C2Ox catalyst exhibits remarkable catalytic activities towards both the pH-universal hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR). Using Rh-SA/Ti3C2Ox as the electrode in the self-driven dual hydrogen production system by combining a Zn-H-2 battery and overall hydrazine splitting units, an ultra-high H-2 generation rate of 45.77 mmol h(-1) can be achieved. Density functional theory calculations indicate that the atomically dispersed single Rh atoms not only make the free energy of adsorbed H (Delta G(*H)) more thermoneutral for the HER but also largely decrease the free-energy barrier of the dehydrogenation of adsorbed NHNH2 for the HzOR.

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