Christian Doppler Laboratory for Sustainable SynGas Chemistry, Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK.
Current address: Department of Chemistry, University of New Hampshire, 23 Academic Way, Durham, NH, 03824, USA.
Angew Chem Int Ed Engl. 2017 Jun 1;56(23):6459-6463. doi: 10.1002/anie.201700949. Epub 2017 May 2.
Single-source precursor syntheses have been devised for the preparation of structurally similar graphitic carbon dots (CDs), with (g-N-CD) and without (g-CD) core nitrogen doping for artificial photosynthesis. An order of magnitude improvement has been realized in the rate of solar (AM1.5G) H evolution using g-N-CD (7950 μmol (g ) h ) compared to undoped CDs. All graphitized CDs show significantly enhanced light absorption compared to amorphous CDs (a-CD) yet undoped g-CD display limited photosensitizer ability due to low extraction of photogenerated charges. Transient absorption spectroscopy showed that nitrogen doping in g-N-CD increases the efficiency of hole scavenging by the electron donor and thereby significantly extends the lifetime of the photogenerated electrons. Thus, nitrogen doping allows the high absorption coefficient of graphitic CDs to be translated into high charge extraction for efficient photocatalysis.
已经设计出了用于制备结构相似的石墨状碳点 (CD) 的单源前体合成方法，其中包括具有 (g-N-CD) 和不具有 (g-CD) 核氮掺杂的 CD，用于人工光合作用。与未掺杂的 CDs 相比，使用 g-N-CD（7950 μmol （g）h）实现了太阳能 (AM1.5G) H 演化速率的数量级提高。与非晶态 CDs (a-CD) 相比，所有石墨化的 CDs 都显示出显著增强的光吸收，但由于光生电荷的提取有限，未掺杂的 g-CD 显示出有限的光敏剂能力。瞬态吸收光谱表明，g-N-CD 中的氮掺杂提高了电子给体清除空穴的效率，从而显著延长了光生电子的寿命。因此，氮掺杂允许石墨状 CD 的高吸收系数转化为高效光催化的高效电荷提取。
