State of the Art and Prospects in Metal–Organic Framework (MOF)-Based and MOF-Derived Nanocatalysis

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 1438 - 1511

Published: June 27, 2019

Metal–organic framework (MOF) nanoparticles, also called porous coordination polymers, are a major part of nanomaterials science, and their role in catalysis is becoming central. The extraordinary variability richness structures afford engineering synergies between the metal nodes, functional linkers, encapsulated substrates, or nanoparticles for multiple selective heterogeneous interactions activations these MOF-based nanocatalysts. Pyrolysis MOF-nanoparticle composites forms highly N- P-doped graphitized MOF-derived that increasingly used as efficient catalysts especially electro- photocatalysis. This review first briefly summarizes this background MOF nanoparticle then comprehensively reviews fast-growing literature reported during last years. parts organic molecular reactions, electrocatalysis, photocatalysis, views prospects. Major challenges our society addressed using well-defined fields synthesis, energy, environment. In spite many achievements, enormous progress still necessary to improve understanding processes involved beyond proof-of-concept, particularly methane oxidation, hydrogen production, water splitting, CO2 reduction methanol, nitrogen fixation, depollution.

Language: Английский

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Homogeneously Catalyzed Electroreduction of Carbon Dioxide—Methods, Mechanisms, and Catalysts

Chemical Reviews, Journal Year: 2018, Volume and Issue: 118(9), P. 4631 - 4701

Published: Jan. 10, 2018

The utilization of CO2 via electrochemical reduction constitutes a promising approach toward production value-added chemicals or fuels using intermittent renewable energy sources. For this purpose, molecular electrocatalysts are frequently studied and the recent progress both in tuning catalytic properties mechanistic understanding is truly remarkable. While earlier years research efforts were focused on complexes with rare metal centers such as Re, Ru, Pd, focus has recently shifted earth-abundant transition metals Mn, Fe, Co, Ni. By application appropriate ligands, these have been rendered more than competitive for compared to heavier homologues. In addition, important roles second outer coordination spheres processes become apparent, metal–ligand cooperativity well-established tool further behavior. Surprising advances also made very simple organocatalysts, although mechanisms behind their reactivity not yet entirely understood. Herein, developments last three decades electrocatalytic homogeneous catalysts reviewed. A discussion underlying principles included along treatment experimental computational techniques studies catalyst benchmarking. Important families discussed detail regard aspects, field highlighted.

Language: Английский

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Homogeneous Catalysis for Sustainable Hydrogen Storage in Formic Acid and Alcohols

Chemical Reviews, Journal Year: 2017, Volume and Issue: 118(2), P. 372 - 433

Published: Oct. 6, 2017

Hydrogen gas is a storable form of chemical energy that could complement intermittent renewable conversion. One the main disadvantages hydrogen arises from its low density, and therefore, efficient handling storage methods are key factors need to be addressed realize hydrogen-based economy. Storage systems based on liquids, in particular, formic acid alcohols, highly attractive carriers as they can made CO2 or other materials, used stationary power units such filling stations, directly transportation fuels. However, bring about paradigm change our infrastructure, catalytic processes release these molecules, well catalysts regenerate molecules hydrogen, required. In this review, we describe considerable progress has been homogeneous catalysis for critical reactions, namely, hydrogenation methanol reverse dehydrogenation reactions. The higher alcohols available feedstocks also described. Key structural features analyzed, role additives, which required many systems. Particular attention paid advances sustainable processes, especially additive-free Earth-abundant metal ions. Mechanistic information presented, it hoped review not only provides an account state art field but offers insights into how superior obtained future.

Language: Английский

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Formic Acid as a Hydrogen Energy Carrier

ACS Energy Letters, Journal Year: 2016, Volume and Issue: 2(1), P. 188 - 195

Published: Dec. 15, 2016

The high volumetric capacity (53 g H2/L) and its low toxicity flammability under ambient conditions make formic acid a promising hydrogen energy carrier. Particularly, in the past decade, significant advancements have been achieved catalyst development for selective generation from acid. This Perspective highlights advantages of this approach with discussions focused on potential applications transportation sector together analysis technical requirements, limitations, costs.

Language: Английский

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First-Row Transition Metal (De)Hydrogenation Catalysis Based On Functional Pincer Ligands

Chemical Reviews, Journal Year: 2018, Volume and Issue: 119(4), P. 2681 - 2751

Published: Dec. 31, 2018

The use of 3d metals in de/hydrogenation catalysis has emerged as a competitive field with respect to "traditional" precious metal catalyzed transformations. introduction functional pincer ligands that can store protons and/or electrons expressed by metal-ligand cooperativity and ligand redox-activity strongly stimulated this development conceptual starting point for rational catalyst design. This review aims at providing comprehensive picture the utilization first-row transition hydrogenation dehydrogenation related synthetic concepts relying on these such hydrogen borrowing methodology. Particular emphasis is put implementation relevance cooperating redox-active within mechanistic scenarios.

Language: Английский

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Recent development of hydrogen and fuel cell technologies: A review

Energy Reports, Journal Year: 2021, Volume and Issue: 7, P. 8421 - 8446

Published: Aug. 27, 2021

Hydrogen has emerged as a new energy vector beyond its usual role an industrial feedstock, primarily for the production of ammonia, methanol, and petroleum refining. In addition to environmental sustainability issues, energy-scarce developed countries, such Japan Korea, are also facing security issue, hydrogen or carriers, ammonia methylcyclohexane, seem be options address these long-term availability issues. China been eagerly developing renewable infrastructure meet their goals growing demand. this review, we focus on electrification through proton-exchange membrane fuel cells (PEMFCs), which widely believed commercially suitable automotive applications, particularly vehicles requiring minimal support, fleets taxies, buses, logistic vehicles. This review covers all key components PEMFCs, thermal water management, related characterization techniques. A special consideration PEMFCs in applications is highlight work, leading development generation, storage, transportation. Furthermore, national strategies toward use reviewed, thereby setting rationale economy.

Language: Английский

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Liquid Organic Hydrogen Carrier (LOHC) – Assessment based on chemical and economic properties

International Journal of Hydrogen Energy, Journal Year: 2019, Volume and Issue: 44(13), P. 6631 - 6654

Published: Feb. 16, 2019

Language: Английский

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A comparative technoeconomic analysis of pathways for commercial electrochemical CO₂ reduction to liquid products

Energy & Environmental Science, Journal Year: 2018, Volume and Issue: 11(6), P. 1536 - 1551

Published: Jan. 1, 2018

Electrochemical reduction of CO₂ to fuels and chemicals is currently a focus significant research effort as technology that can simultaneously mitigate greenhouse gas emissions while storing renewable electricity for use on demand. Herein, the economics select liquid products analyzed.

Language: Английский

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Electrochemical CO2 reduction to high-concentration pure formic acid solutions in an all-solid-state reactor

Nature Communications, Journal Year: 2020, Volume and Issue: 11(1)

Published: July 20, 2020

Electrochemical CO2 reduction reaction (CO2RR) to liquid fuels is currently challenged by low product concentrations, as well their mixture with traditional electrolytes, such KHCO3 solution. Here we report an all-solid-state electrochemical CO2RR system for continuous generation of high-purity and high-concentration formic acid vapors solutions. The cathode anode were separated a porous solid electrolyte (PSE) layer, where electrochemically generated formate proton recombined form molecular acid. can be efficiently removed in the via inert gas stream flowing through PSE layer. Coupling high activity (formate partial current densities ~450 mA cm-2), selectivity (maximal Faradaic efficiency ~97%), stability (100 hours) grain boundary-enriched bismuth catalyst, demonstrated ultra-high concentrations pure solutions (up nearly 100 wt.%) condensed from flexible tuning carrier stream.

Language: Английский

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Reduced SnO₂ Porous Nanowires with a High Density of Grain Boundaries as Catalysts for Efficient Electrochemical CO₂‐into‐HCOOH Conversion

Angewandte Chemie International Edition, Journal Year: 2017, Volume and Issue: 56(13), P. 3645 - 3649

Published: Feb. 23, 2017

Abstract Electrochemical conversion of CO 2 into energy‐dense liquids, such as formic acid, is desirable a hydrogen carrier and chemical feedstock. SnO x one the few catalysts that reduce acid with high selectivity but at overpotential low current density. We show an electrochemically reduced porous nanowire catalyst (Sn‐pNWs) density grain boundaries (GBs) exhibits energy efficiency ‐into‐HCOOH higher than analogous catalysts. HCOOH formation begins lower (350 mV) reaches steady Faradaic ca. 80 % only −0.8 V vs. RHE. A comparison commercial nanoparticles confirms improved reduction performance Sn‐pNWs due to GBs within structure, which introduce new catalytically active sites. Produced scalable plasma synthesis technology, have potential for application in industry.

Language: Английский

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