Formic acid as H<sub>2</sub>storage system: hydrogenation of CO<sub>2</sub>and decomposition of formic acid by solid molecular phosphine catalysts

Kipshagen, Anna; Baums, Janine C.; Hartmann, Heinrich; Besmehn, Astrid; Hausoul, Peter J. C.; Palkovits, Regina

doi:10.1039/d2cy00608a

Cited by 5 publications

(3 citation statements)

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“…tions of NMR shifts were performed with the ORCA code version 5.0.1. [3,4] Geometry of the model was optimized at the revPBE-D4/pcseg-1 level of theory [5][6][7][8] and NMR shieldings were subsequently calculated at the DSD-PBEP86/pcSseg-1 level of theory [9,10] with the GIAO approach [11] employing RIJCOSX approximation and the cc-pwCVDZ/C and def2/J auxiliary basis sets. [12][13][14] Calculated NMR shieldings were converted into isotropic chemical shifts using CH 4 and N 2 molecules in the gas phase as references.…”

Section: Methodsmentioning

confidence: 99%

“…[ 10 ] FA is a valuable and safe chemical reagent with non‐corrosive, eco‐friendly properties. [ 11 ] It is mainly used in the leather/textile industry, pharmaceuticals, and food industry. Contrary to methanol which is another one‐carbon product of CO 2 RR, FA does not cross over the polymer membranes and is not causing blindness.…”

Section: Introductionmentioning

confidence: 99%

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Enhanced Solar CO₂ Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Kaya

Ditz

Jaworski

et al. 2023

Advanced Sustainable Systems

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The immobilization and structural analysis of platinum nanoparticles on a nitrogen‐rich, bipyridine‐containing covalent triazine framework (bpyCTF) having structural defects are disclosed by taking advantage of 15N solid‐state nuclear magnetic resonance measurements at natural 15N isotope abundance and X‐ray photoelectron spectroscopic analyses. The photocatalyst (Pt@bpyCTF) with structural defects reduces CO2 to formic acid (FA) at a rate of 152 µmol h−1g−1 and a selectivity higher than 95% over CO and H2 in water under simulated solar light. The presence of amine defects and the immobilization of Pt cause improvement in the photocurrent density and CO2 capture capacity (≈8% by weight) despite the moderate surface area (0.54 cm3 g−1)of the photocatalyst. Theoretical models and density functional theory calculations are employed to investigate the possible CO2 reduction reaction (CO2RR) mechanisms. Considering the exceptional CO2 capture capacity and high FA production using only CO2‐bubbled water, this work highlights the great potential of nitrogen‐rich CTFs for photocatalyzed CO2RRs under green conditions.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Enhanced Solar CO₂ Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Kaya

Ditz

Jaworski

et al. 2023

Advanced Sustainable Systems

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“…It is highly desired to develop a catalyst that can concomitantly catalyze the hydrogenation and dehydrogenation processes for a hydrogen cycle system. Although homogeneous catalysts exhibit superior catalytic activity, disadvantages, such as the use of expensive ligands and inseparability from the catalytic system, seriously restrict their industrial applications [74][75][76][77]. In contrast, heterogeneous catalysts possess significant advantages in product separation, recycling, and continuous operation, providing prospects for their industrial applications [78][79][80][81][82].…”

Section: Activated Carbon-supported Monometallic Catalystsmentioning

confidence: 99%

Application of Heterogeneous Catalysis in Formic Acid-Based Hydrogen Cycle System

Wang,

Qian,

Sun

et al. 2023

Catalysts

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H2 has aroused significant attention as an unpolluted and renewable energy carrier. However, the efficient storage and controllable release of H2 are urgent to be addressed. Through the hydrogenation of CO2 (bicarbonate) to produce formic acid (formate) and reverse dehydrogenation reactions, a carbon-neutral formic acid-based hydrogen cycle system can be established. Given the excellent recyclability and facile separation of heterogeneous catalysis, the development of heterogeneous catalysts for these reversible interconversions is thoroughly summarized, with a special focus on the structure–activity relationship and the mechanistic insight. Finally, the challenges and opportunities surrounding the formic acid-based hydrogen cycle system are discussed. It is hoped that this review will provide guidance and an idea for the design and development of efficient heterogeneous catalysts for the carbon-neutral H2 storage and release system.

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Electrochemical reduction of CO2: A roadmap to formic and acetic acid synthesis for efficient hydrogen storage

Orlić,

Hochenauer,

Nagpal

et al. 2024

Energy Conversion and Management

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Formic acid as H₂storage system: hydrogenation of CO₂and decomposition of formic acid by solid molecular phosphine catalysts

Abstract: The synthesis and decomposition of formic acid (FA) in aqueous triethylamine (NEt3) with solid molecular phosphine catalysts is demonstrated. Ru-catalyst based on the polymeric analog of 1,2-bis(diphenylphosphino)ethane presented the highest...

Cited by 5 publications

References 51 publications

Enhanced Solar CO₂ Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Enhanced Solar CO₂ Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Application of Heterogeneous Catalysis in Formic Acid-Based Hydrogen Cycle System

Electrochemical reduction of CO2: A roadmap to formic and acetic acid synthesis for efficient hydrogen storage

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Formic acid as H2storage system: hydrogenation of CO2and decomposition of formic acid by solid molecular phosphine catalysts

Abstract: The synthesis and decomposition of formic acid (FA) in aqueous triethylamine (NEt3) with solid molecular phosphine catalysts is demonstrated. Ru-catalyst based on the polymeric analog of 1,2-bis(diphenylphosphino)ethane presented the highest...

Cited by 5 publications

References 51 publications

Enhanced Solar CO2 Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Enhanced Solar CO2 Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Application of Heterogeneous Catalysis in Formic Acid-Based Hydrogen Cycle System

Electrochemical reduction of CO2: A roadmap to formic and acetic acid synthesis for efficient hydrogen storage

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Product

Resources

About

Formic acid as H₂storage system: hydrogenation of CO₂and decomposition of formic acid by solid molecular phosphine catalysts

Enhanced Solar CO₂ Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects

Enhanced Solar CO₂ Photoreduction to Formic Acid by Platinum Immobilization on Bipyridine Covalent Triazine Framework with Defects