The development of an artificial heterogeneous dyad by covalently anchoring a hydrogen-evolving molecule catalyst to a semiconductor photosensitizer through a bridging ligand is highly challenging. Herein, we adopt the inorganic-organic hybrid CdS-DETA NSs (DETA= diethylenetriamine, NSs= nanosheets) as initial matrix to successfully construct an imine bond (-CH= N-) linked heterogeneous dyad CdS-N=CH-Ni through the condensation reaction between the amino groups of CdS-DETA and the aldehyde group of the water reduction molecular catalyst, (tpy-CHO)(2)NiCl-2 (tpy=terpyridine). The CdS-N= CH-Ni enables a turnover number (TON) of about 43815 versus Ni catalysts and an initial turnover frequency (TOF) of approximately 0.47 s(-1) in 26h under visible-light irradiation (lambda > 420 nm). The apparent quantum yield (AQY) reaches (9.9 +/- 0.8) at 420 nm. Under optical conditions, the CdS-N=CH-Ni can achieve a considerable amount of hydrogen production, 507.1 +/- 27 mu mol H-2 for 6 h, which is 1.27 times that generated from the mechanically mixed system of CdS-DETA NSs and (tpy-CH= NR)(2)NiCl-2 (III) under otherwise identical conditions. Furthermore, its TON value based on Ni species is also higher than that of the mixed system of CdS-DETA and III.
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