Hydrogenation of CO2 or CO2 Derivatives to Methanol under Molecular Catalysis: A Review

Xue, Wenxuan; Tang, Conghui

doi:10.3390/en15062011

Cited by 14 publications

(3 citation statements)

References 68 publications

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“… There have been various metal complexes that can catalyze the regioselective reduction of NAD(P) + to produce NAD(P)H . There have also been a number of metal complexes that can catalyze the CO 2 reduction by H 2 . – Thus, the further combination of molecular models of PSI and PSII with NAD(P) + reduction catalysts may make it possible to achieve artificial photosynthesis in which NAD(P)H is produced from H 2 O under visible light irradiation. The combination of molecular models of PSI and PSII with CO 2 reduction catalysts may also make it possible to reduce CO 2 to solar fuels such as CO, HCO 2 H, CH 3 OH, and CH 4 .…”

Section: Discussionmentioning

confidence: 99%

Reaction Intermediates in Artificial Photosynthesis with Molecular Catalysts

et al. 2022

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In nature, water oxidation is catalyzed by Mn4Ca clusters in the oxygen-evolving complex (OEC) of photosystem II (PSII), in which a manganese(V)-oxo species acts as an active reaction intermediate. Electrons and protons taken from water in PSII are used to reduce plastoquinone to plastoquinol via photoinduced charge separation in the photosynthetic reaction center. In photosystem I (PSI), NADP+ coenzyme is reduced by plastoquinol via photoinduced charge separation in the photosynthetic reaction center to produce NADPH, which is used as a reductant to reduce CO2 to carbohydrates in the Calvin cycle. Extensive efforts have so far been made to mimic functions of PSII and PSI for photocatalytic water oxidation and reduction to produce O2 and H2, respectively. Characterization and reactivity of high-valent metal-oxo, -hydroperoxo, -peroxo, and -superoxo intermediates have been investigated to clarify the mechanisms of water oxidation. Metal hydride complexes have also been studied in relation with the catalytic reactivity for water reduction to produce H2 as well as NAD+ reduction to NADH. This Review is intended to provide an overview on the functional model reactions of PSII and PSI for the photocatalytic water oxidation and reduction, respectively. The roles of high-valent metal-oxo, -hydroperoxo, -peroxo, and -superoxo complexes as the reaction intermediates in photocatalytic water oxidation are focused in relation with the catalytic mechanisms of water oxidation. The roles of metal hydride complexes are also discussed in relation with the catalytic mechanisms of hydrogen evolution and NAD+ reduction to NADH. The combination of functional model reactions of PSII and PSI leads to construct molecular artificial photosynthetic systems in which water is split to H2 and O2 in a 2:1 ratio, providing a way to realize artificial photosynthesis in molecular levels.

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Section: Discussionmentioning

confidence: 99%

Reaction Intermediates in Artificial Photosynthesis with Molecular Catalysts

et al. 2022

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“…27 The latter material is an excellent support in transforming homogeneous catalysts into heterogeneous ones. MOFs are a class of materials that have gained traction in various applications, 17 and can be used as excellent support materials in the development of single site catalysts. 18 These materials can be developed by tuning-based design, a retrosynthesis approach in designing MOFs that enables structural tuning for specific applications.…”

Section: Introductionmentioning

confidence: 99%

A single site catalyst supported in mesoporous UiO-66 for catalytic conversion of carbon dioxide to formate

Gumbo,

Ocansey,

Makhubela

et al. 2024

Sustainable Energy Fuels

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“…The production of FA is crucial as it is projected to become an outstanding hydrogen carrier in fuel cells vital for the 21st century society. , Its inordinate advantages are high volumetric hydrogen density, high chemical stability, easier storage, and low toxicity. , Efficient CO 2 capture and conversion to FA under ambient hydrogenation conditions are extremely important and could result in a truly carbon-neutral liquid fuel. , …”

Section: Introductionmentioning

confidence: 99%

Hydrogenation of Carbon Dioxide to Formate by Noble Metal Catalysts Supported on a Chemically Stable Lanthanum Rod-Metal–Organic Framework

et al. 2023

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The conversion of carbon dioxide to formate is of great importance for hydrogen storage as well as being a step to access an array of olefins. Herein, we have prepared a JMS-5 metal–organic framework (MOF) using a bipyridyl dicarboxylate linker, with the molecular formula [La2(bpdc)3/2(dmf)2(OAc)3]·dmf. The MOF was functionalized by cyclometalation using Pd(II), Pt(II), Ru(II), Rh(III), and Ir(III) complexes. All metal catalysts supported on JMS-5 showed activity for CO2 hydrogenation to formate, with Rh(III)@JMS-5a and Ir(III)@JMS-5a yielding 4319 and 5473 TON, respectively. X-ray photoelectron spectroscopy of the most active catalyst Ir(III)@JMS-5a revealed that the iridium binding energies shifted to lower values, consistent with formation of Ir–H active species during catalysis. The transmission electron microscopy images of the recovered catalysts of Ir(III)@JMS-5a and Rh(III)@JMS-5a did not show any nanoparticles. This suggests that the catalytic activity observed was due to Ir(III) and Rh(III). The high activity displayed by Ir(III)@JMS-5a and Rh(III)@JMS-5a compared to using the Ir(III) and Rh(III) complexes on their own is attributed to the stabilization of the Ir(III) and Rh(III) on the nitrogen and carbon atom of the MOF backbone.

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Hydrogenation of CO2 or CO2 Derivatives to Methanol under Molecular Catalysis: A Review

Cited by 14 publications

References 68 publications

Reaction Intermediates in Artificial Photosynthesis with Molecular Catalysts

Reaction Intermediates in Artificial Photosynthesis with Molecular Catalysts

A single site catalyst supported in mesoporous UiO-66 for catalytic conversion of carbon dioxide to formate

Hydrogenation of Carbon Dioxide to Formate by Noble Metal Catalysts Supported on a Chemically Stable Lanthanum Rod-Metal–Organic Framework

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