A Porphyrin‐Doped Polymer Catalyzes Selective, Light‐Assisted Water Oxidation in Seawater

Chen, Jun; Wagner, Paweł; Tong, Lei; Wallace, Gordon G.; Officer, David L.; Swiegers, Gerhard F.

doi:10.1002/anie.201107355

Cited by 43 publications

(58 citation statements)

References 23 publications

(22 reference statements)

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“…The mechanism of light-assisted catalysis in PEDOT-1 is likely similar to that identied in the previous study involving poly(terthiophene), 14 namely, light absorption by 1, followed by electron injection from 1 into the PEDOT matrix. At the applied voltage, the resulting reduced form of PEDOT would be immediately oxidized by the electrode, creating charge separation.…”

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confidence: 65%

A light-assisted, polymeric water oxidation catalyst that selectively oxidizes seawater with a low onset potential

et al. 2013

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Vapour phase polymerisation (vpp) of PEDOT to incorporate high levels of a sulphonated manganese porphyrin yields a vivid green conducting polymer that, under illumination, catalyzes selective oxidation of water from seawater from ca. 0.40 V (vs. NHE; Pt counter electrode) without observable chlorine formation. This onset potential is comparable to that of certain metal oxide semiconductors that achieve higher photocurrents but are not capable of selectively oxidising the water in seawater. A light-assisted, polymeric water oxidation catalyst that selectively oxidizes seawater with a low onset potential † Jun Chen, * Pawel Wagner, Lei Tong, Danijel Boskovic, Weimin Zhang, David Officer, Gordon G. Wallace and Gerhard F. Swiegers * Vapour phase polymerisation (vpp) of PEDOT to incorporate high levels of a sulphonated manganese porphyrin yields a vivid green conducting polymer that, under illumination, catalyzes selective oxidation of water from seawater from ca. 0.40 V (vs. NHE; Pt counter electrode) without observable chlorine formation. This onset potential is comparable to that of certain metal oxide semiconductors that achieve higher photocurrents but are not capable of selectively oxidising the water in seawater.

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confidence: 65%

A light-assisted, polymeric water oxidation catalyst that selectively oxidizes seawater with a low onset potential

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“…Because the water oxidation is a ratelimiting step, the positive shift of the VB in 3DOM g-C 3 N 4 -PW 11 facilitates to overcome the kinetic barrier of the O 2 evolution. Moreover, the CB level in 3DOM g-C 3 N 4 -PW 11 (−0.04 V vs. NHE) is more positive than the one-electron reduction of O 2 to •OOH (−0.13 V vs. NHE), and has sufficient potential difference (0.73 V) from the twoelectron reduction of O 2 to H 2 O 2 (0.69 V vs. NHE) [42]. The results are in accordance with the reported g-C 3 N 4 -PDI and g-C 3 N 4 -NiFeO catalysts, in which both the CB and VB levels of g-C 3 N 4 -PDI and g-C 3 N 4 -NiFeO are shifted positively [6e,32].…”

Section: −2mentioning

confidence: 98%

Covalent combination of polyoxometalate and graphitic carbon nitride for light-driven hydrogen peroxide production

et al. 2017

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A B S T R A C TThe polyoxometalate (POM) cluster of [PW 11 O 39 ] 7-(PW 11 ) has been successfully covalent combined with the three dimensionally ordered macroporous graphitic carbon nitride (3DOM g-C 3 N 4 ) through the organic linker strategy. The characterization such as solid-state NMR and XPS results confirm the organosilicon agent of (triethoxysilyl)-propyl isocyanate can act as the linker to covalent combine the PW 11 cluster with 3DOM g-C 3 N 4 . The hybrid catalyst of 3DOM g-C 3 N 4 -PW 11 exhibits efficient catalytic performance (2.4 μmol h −1 ) for lightdriven H 2 O 2 production from H 2 O and O 2 in the absence of organic electron donors. The ESR results suggest that one-electron reduction of O 2 to •OOH is indeed suppressed over 3DOM g-C 3 N 4 -PW 11 . Furthermore, the Koutecky-Levich plot obtained from electrochemical rotating disk electrode (RDE) analysis of oxygen reduction reaction (ORR) for 3DOM g-C 3 N 4 -PW 11 reveals the value of electron transfer during the ORR process is 2.30, indicating the covalent combination can promote the two-electron O 2 reduction. In addition, the recycle experiment results reveal that the heterogeneous 3DOM g-C 3 N 4 -PW 11 is catalytic stable.

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“…The only other catalyst known to be capable to selectively oxidizing water in seawater is the biological catalyst of photosynthesis, the photosystem II water oxidizing complex (PSII-WOC), that is present in marine and hypersaline organisms. Given that water oxidation catalysts are known to operate by either a bimolecular or monomolecular (nucleophilic attack) mechanism, the observed absence of HClO, which spontaneously equilibrates to form Cl 2 in water, and which should have been formed in the presence of chloride ions, was inferred to indicate a cooperative bimolecular mechanism similar to that in 8 [76]. No physical evidence was available, however, showing catalytic interactions between monomeric porphyrins.…”

Section: Scheme 18 Hydrogen-generating Catalysts (Reproduced With Pmentioning

confidence: 99%

Kinematic molecular manufacturing machines

Boskovic

Balakrishnan

Huang

et al. 2016

Coordination Chemistry Reviews

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The principles of kinematic manufacturing machines of the type widely used since the industrial revolution are reviewed. Consideration is then given to how the principles of kinematics ('the geometry of motion') may manifest in molecular catalysts. Actions of this type involve synchronized, regular, repeated and rapid conformational flexing along geometrically optimum pathways that define a single degree of freedom. The proposition that many of the catalysts of biology, enzymes, may generally exploit a kinematic action is discussed. Thereafter, in the major portion of this work, representative abiological molecular catalysts whose actions display the characteristic features of kinematic manufacturing processes, are reviewed. In accordance with the principles of kinematics, molecular catalytic actions of this type are shown to be capable of transforming unremarkable chemical species into powerful catalysts with high activities, selectivities, and durabilities. Disciplines Engineering | Physical Sciences and Mathematics Engineering, Wenzhou University, Wenzhou 325027, Peoples Republic of ChinaAbstract: The principles of kinematic manufacturing machines of the type widely used since the industrial revolution are reviewed. Consideration is then given to how the principles of kinematics ('the geometry of motion') may manifest in molecular catalysts. Actions of this type involve synchronized, regular, repeated and rapid conformational flexing along geometrically optimum pathways that define a single degree of freedom. The proposition that many of the catalysts of biology, enzymes, may generally exploit a kinematic action is discussed. Thereafter, in the major portion of this work, representative abiological molecular catalysts whose actions display the characteristic features of kinematic manufacturing processes, are reviewed. In accordance with the principles of kinematics, molecular catalytic actions of this type are shown to be capable of transforming unremarkable chemical species into powerful catalysts with high activities, selectivities, and durabilities.

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A Porphyrin‐Doped Polymer Catalyzes Selective, Light‐Assisted Water Oxidation in Seawater

Cited by 43 publications

References 23 publications

A light-assisted, polymeric water oxidation catalyst that selectively oxidizes seawater with a low onset potential

A light-assisted, polymeric water oxidation catalyst that selectively oxidizes seawater with a low onset potential

Covalent combination of polyoxometalate and graphitic carbon nitride for light-driven hydrogen peroxide production

Kinematic molecular manufacturing machines

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