Abstract
The catalytic tetranuclear manganese-calcium-oxo cluster in the photosynthetic reaction center, photosystem II, provides an excellent blueprint for light-driven water oxidation in nature. The water oxidation reaction has attracted intense interest due to its potential as a renewable, clean, and environmentally benign source of energy production. Inspired by the oxygen-evolving complex of photosystem II, a large of number of highly innovative synthetic bio-inspired molecular catalysts are being developed that incorporate relatively cheap and abundant metals such as Mn, Fe, Co, Ni, and Cu, as well as Ru and Ir, in their design. In this review, we briefly discuss the historic milestones that have been achieved in the development of transition metal catalysts and focus on a detailed description of recent progress in the field.
Highlights
Photosystem II is comprised of a core of heterodimeric polypeptides, D1 and D2, surrounded by ~20 polypeptide subunits [14], within which there are more than 1300 water molecules [10]
The challenges in designing efficient artificial catalysts stem from the complexity of the water oxidation reaction, which requires the transfer of four electrons and four protons during the catalytic cycle [7,36,37]
Further improvements in the design of dinuclear ruthenium catalysts included the incorporation of a rigid polypyridyl equatorial ligand in [RuII2(μ-L)(μ-Cl)(pic)4]3+ (8) (where L = 6-di-(6 -[1,8 -naphthyrid-2 -yl]-pyridin-2 -yl)pyrazine and pic = 4-picoline), which improved the catalytic performance for chemical water oxidation using chemical oxidation of water using [Ce(NO3)6][(NH4)2] (CAN) as a sacrificial oxidant at pH 1 with a turnover number (TON) and turnover frequency (TOF) of 538 [50,79] and 0.046 s−1, respectively [50,71]
Summary
Green, sustainable, and renewable source of energy, the photochemical conversion and storage of solar energy has been a challenge [1]. The challenges in designing efficient artificial catalysts stem from the complexity of the water oxidation reaction, which requires the transfer of four electrons and four protons during the catalytic cycle [7,36,37]. This is a major bottleneck, as an effective catalyst would have to accommodate successive charge storage states and participate in PCET reactions during water oxidation [4,23,29,38]. FtFtdhhiiegegevuudedrrleeeoesspi22igge..ndnTTohhfoofeefrs33syeddynanc(t(hMMthhemenntit,,cieFcFtbaeebil,,oiCCao-ir-oonei,,nsaNNpslpisiiro,,ieraadesnndhmddomwCoClouunel).)ce,,uc44ulddalra((rcRRaucutaa)),t,layaalsnnytddsstfs55oddfro((wrIIrraw))tmmearteeeottraaxlloissdxiiainndtiattohhtnieeo. pnpK.eeerrKyiiooeeddyxiiaccemxttaaapbbmllleeepslttoehhsfaatttohhhfeaaccvvaaeettaabbllyeeyseestnntssiitnnthhccaaoottrrphphoaoavrvraaeetteebbddeeeeiinnnn developed for each metal are shown
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