Knitting the Catalytic Pattern of Artificial Photosynthesis to a Hybrid Graphene Nanotexture
详细信息 查看全文
- 作者：Mildred Quintana ; Alejandro Montellano L贸pez ; Stefania Rapino ; Francesca Maria Toma ; Matteo Iurlo ; Mauro Carraro ; Andrea Sartorel ; Chiara Maccato ; Xiaoxing Ke ; Carla Bittencourt ; Tatiana Da Ros ; Gustaaf Van Tendeloo ; Massimo Marcaccio ; Francesco Paolucci ; Maurizio Prato ; Marcella Bonchio
- 刊名：ACS Nano
- 出版年：2013
- 出版时间：January 22, 2013
- 年：2013
- 卷：7
- 期：1
- 页码：811-817
- 全文大小：487K
- 年卷期：v.7,no.1(January 22, 2013)
- ISSN：1936-086X
文摘
The artificial leaf project calls for new materials enabling multielectron catalysis with minimal overpotential, high turnover frequency, and long-term stability. Is graphene a better material than carbon nanotubes to enhance water oxidation catalysis for energy applications? Here we show that functionalized graphene with a tailored distribution of polycationic, quaternized, ammonium pendants provides an sp2 carbon nanoplatform to anchor a totally inorganic tetraruthenate catalyst, mimicking the oxygen evolving center of natural PSII. The resulting hybrid material displays oxygen evolution at overpotential as low as 300 mV at neutral pH with negligible loss of performance after 4 h testing. This multilayer electroactive asset enhances the turnover frequency by 1 order of magnitude with respect to the isolated catalyst, and provides a definite up-grade of the carbon nanotube material, with a similar surface functionalization. Our innovation is based on a noninvasive, synthetic protocol for graphene functionalization that goes beyond the ill-defined oxidation鈥搑eduction methods, allowing a definite control of the surface properties.