Chandrasekaran Soundarrajan, Kaeffer Nicolas, Cagnon Laurent, Aldakov Dmitry, Fize Jennifer, Nonglaton Guillaume, Baleras François, Mailley Pascal, Artero Vincent
Université Grenoble Alpes , CNRS , CEA , Laboratoire de Chimie et Biologie des Métaux , 17 rue des Martyrs , 38000 Grenoble , France . Email:
Université Grenoble Alpes , CEA-LETI/DTBS , Laboratoire Chimie , Capteurs et Biomatériaux , 17 rue des Martyrs , 38000 Grenoble , France.
Chem Sci. 2019 Mar 12;10(16):4469-4475. doi: 10.1039/c8sc05006f. eCollection 2019 Apr 28.
Hydrogen production through direct sunlight-driven water splitting in photo-electrochemical cells (PECs) is a promising solution for energy sourcing. PECs need to fulfill three criteria: sustainability, cost-effectiveness and stability. Here we report an efficient and stable photocathode platform for H evolution based on Earth-abundant elements. A p-type silicon surface was protected by atomic layer deposition (ALD) with a 15 nm TiO layer, on top of which a 300 nm mesoporous TiO layer was spin-coated. The cobalt diimine-dioxime molecular catalyst was covalently grafted onto TiO through phosphonate anchors and an additional 0.2 nm ALD-TiO layer was applied for stabilization. This assembly catalyzes water reduction into H in phosphate buffer (pH 7) with an onset potential of +0.47 V RHE. The resulting current density is -1.3 ± 0.1 mA cm at 0 V RHE under AM 1.5 solar irradiation, corresponding to a turnover number of 260 per hour of operation and a turnover frequency of 0.071 s.
通过光电化学电池（PEC）中直接阳光驱动的水分解来制氢是一种很有前景的能源解决方案。PEC需要满足三个标准：可持续性、成本效益和稳定性。在此，我们报告了一种基于储量丰富的元素的高效且稳定的用于析氢的光电阴极平台。通过原子层沉积（ALD）用15纳米的TiO层保护p型硅表面，在其顶部旋涂300纳米的介孔TiO层。通过膦酸酯锚将钴二亚胺二肟分子催化剂共价接枝到TiO上，并施加额外的0.2纳米ALD-TiO层用于稳定。该组件在磷酸盐缓冲液（pH 7）中将水还原为氢气，起始电位为+0.47 V（相对于可逆氢电极）。在AM 1.5太阳辐照下，在0 V（相对于可逆氢电极）时，所得电流密度为-1.3±0.1 mA/cm²，对应于每小时运行260的周转数和0.071 s⁻¹的周转频率。
