Formic Acid‐Based Liquid Organic Hydrogen Carrier System with Heterogeneous Catalysts

Zhong, Heng; Iguchi, Masayuki; Chatterjee, Maya; Himeda, Yuichiro; Xu, Qiang; Kawanami, Hajime

doi:10.1002/adsu.201700161

Cited by 143 publications

(110 citation statements)

References 123 publications

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“…[100,101] Thus, high-pressure gas generation by FADH, especially over 35 MPa to charge highpressure hydrogen into the fuel cell vehicle (FCV) is another important target of our studies. However, heterogeneous catalysts show lower activity than homogeneous catalysts.…”

Section: Wwwadvancedsciencenewscommentioning

confidence: 99%

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Onishi

Iguchi

Yang

et al. 2018

Advanced Energy Materials

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112

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We are engaged in research and development to reduce CO 2 emissions. Longterm increase of CO 2 concentration in the atmosphere has a great influence on climate change. [1] Therefore, developing technologies aiming to reduce CO 2 emissions and to overcome the present society depending on fossil fuels as primary energy. Additionally, transition of fossil fuels into renewable energies is also important for realizing future sustainable society. [2] The most suitable material for this goal is considered to be hydrogen, because its combustion emits only water as a byproduct. In addition, hydrogen possesses almost three times as much energy as natural gases, and can supply electric power very efficiently for fuel cells without releasing greenhouse gases and air pollutants. [3] However, hydrogen also has serious drawbacks for practical applications. Most serious problem is that, hydrogen forms as a gas at ambient conditions with very low density (0.0899 kg m −3 at 0 °C, 0.10 MPa) over ten times lower than air (1.293 kg m −3 at 0 °C, 0.10 MPa). As a result, it becomes difficult to store and transport hydrogen safely. Developing safe and efficient hydrogen storage materials is one of the most difficult challenges for the transformation from the fossil fuel-based economy to hydrogen-based one as a long-term solution for a safe energy future.Hydrogen has attracted considerable attention as an energy source, and various attempts to develop suitable methods for hydrogen generation are made at the National Institute of Advanced Industrial Science and Technology. In this paper, the authors introduce their recent strategies to store hydrogen using formic acid (FA) as a hydrogen carrier. FA, which is believed to be one of the most promising liquid organic hydrogen carriers, can provide a viable method for safe hydrogen transportation. In order to optimize the performance of hydrogen storage with FA, the authors have investigated both homogeneous and heterogeneous catalysts. For example, Ir catalysts anchoring N^N-bidentate ligands show high catalytic activity for both the reactions of FA synthesis and hydrogen generation from FA. Ultrafine Pd-based nanoparticles are also immobilized on various supports, which show excellent catalytic performance for FA dehydrogenation under mild conditions. The authors also develop both homogeneous and heterogeneous catalysts to generate high-pressure gases (H 2 and CO 2 ) over 120 and 35 MPa, respectively,

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Section: Wwwadvancedsciencenewscommentioning

confidence: 99%

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Onishi

Iguchi

Yang

et al. 2018

Advanced Energy Materials

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112

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“…[1,2] Homogeneous catalysts have been developed for CO 2 reduction under both electrochemical and photochemical conditions. These competent catalysts transform CO 2 into formic acid with high selectivity and turnover number.Aproposed mechanism, with combined electron transfer and catalytic cycles, models the experimental rate of formic acid production.…”

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“…[1,2] Homogeneous catalysts have been developed for CO 2 reduction under both electrochemical and photochemical conditions. Success in this endeavor requires confronting the inherent stabilitya nd low thermodynamic value of CO 2 and would transform this ubiquitous waste product into av aluable feedstock.…”

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“…[Ru{k 3 -2,6-{Ph 2 PNR} 2 (NC 5 H 3 )}(CO) 2 Cl + ]Cl À (R = H, Me), are, to our knowledge,t he first Ru-based photocatalystsf or CO 2 reduction that do not possess a-diimine ligation as well as use ap incer ligand framework. [Ru{k 3 -2,6-{Ph 2 PNR} 2 (NC 5 H 3 )}(CO) 2 Cl + ]Cl À (R = H, Me), are, to our knowledge,t he first Ru-based photocatalystsf or CO 2 reduction that do not possess a-diimine ligation as well as use ap incer ligand framework.…”

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“…The direct addition of N,N'-bis(diphenylphosphino)-2,6-di-(methylamino)pyridine to [{Ru(CO) 3 Cl 2 } 2 ]i nt oluene followed by heatinga t1 00 8Cu nder N 2 for 16 hl ed to the new cationic Ru complex [Ru{k 3 -2,6-(Ph 2 PNMe) 2 NC 5 H 3 }(CO) 2 Cl] + Cl À (1 + + Cl À )a sa colorless solid with ay ield of 89 %. Replacing the starting ligand with N,N'-bis(diphenylphosphino)-2,6-diaminopyridine and followingasimilar procedure produced the analogous complex,…”

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Visible‐Light Photocatalytic Reduction of CO₂ to Formic Acid with a Ru Catalyst Supported by N,N′‐Bis(diphenylphosphino)‐2,6‐diaminopyridine Ligands

et al. 2019

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Visible-light photocatalytic CO 2 reduction is carried out by using aR u II complex supportedb yN,N'-bis(diphenylphosphino)-2,6-diaminopyridine( "PNP")l igands, an unprecedented molecular architecture for this reaction that breaks the longstanding domination of a-diimine ligands. These competent catalysts transform CO 2 into formic acid with high selectivity and turnover number.Aproposed mechanism, with combined electron transfer and catalytic cycles, models the experimental rate of formic acid production.Designing and assembling catalysts that can utilize the energy of visible light to overcome the barriers to reduce CO 2 is an important fundamentala nd technological challenge. Success in this endeavor requires confronting the inherent stabilitya nd low thermodynamic value of CO 2 and would transform this ubiquitous waste product into av aluable feedstock. For example, photocatalytic formation of formic acid, at wo-electron reductionp roduct of CO 2 ,w ould yield ac ommodity chemical and al iquid fuel. Furthermore, formic acid has been identified and explored as ap otential carrier of dihydrogen. [1,2] Homogeneous catalysts have been developed for CO 2 reduction under both electrochemical and photochemical conditions. [3][4][5][6] Photocatalysis is ap articularly appealing approacha s it relies on an essentially limitless and clean solar energy source.P hotocatalytic systemsc onsisto fi ntegrated components that include ap hotosensitizer (PS)f or harvesting the energy of the light, an electron donor (ED)t hat provides electrons for the reduction, and ac atalyst (CAT)t hat is as ite for the transformation of CO 2 .T oo ur knowledge,s ince their discovery in 1985, [7] all of the reported molecular photocatalysts based on Ru II have used a-diimine supporting ligandsa nd these speciesh ave fallen into two broad groups.O ne class are bis(a-diimine) speciesr epresentedb ycis-[Ru(N^N) 2 (CO) 2 ] 2 + [8][9][10][11] and the other are mono(a-diimine) catalysts represented by cis,trans-[Ru(N^N)(CO) 2 Cl 2 ]. [12][13][14] Althoughavariety of substituents on the a-diimine ligands have been productively explored to improvec atalystp erformance, given the maturity of this field, ab roader variationo fm olecular architecture is required to provide new insights and stimulate new concepts in this field. Ligand variation and discoverya re ac entral challenge in catalysis and expanding Ru-based photocatalysts beyond the restrictions of a-diimine support is certainly warranted. Support for this approachc omes from av ery recent report on the use of ap hotocatalytic phosphine-substituted Ru II terpyridine complex-trans-[Ru(tpy)(8-quinolyl(diphenyl)phosphine)-(MeCN)] 2 + -that functions as both ap hotosensitizer andacatalyst for CO 2 reduction. [15,16] Recently,p incer ligand-supported catalysts of Fe, Co, Ru, and Ir have been shown to have excellent activity and selectivity for hydrogenation of CO 2 . [17][18][19][20][21][22][23] Pincer-supported ruthenium complexes can catalyze hydrogenation of CO 2 to yield formate, as wella st he ...

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Nanopore‐Supported Metal Nanocatalysts for Efficient Hydrogen Generation from Liquid‐Phase Chemical Hydrogen Storage Materials

et al. 2020

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Formic Acid‐Based Liquid Organic Hydrogen Carrier System with Heterogeneous Catalysts

Cited by 143 publications

References 123 publications

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Visible‐Light Photocatalytic Reduction of CO₂ to Formic Acid with a Ru Catalyst Supported by N,N′‐Bis(diphenylphosphino)‐2,6‐diaminopyridine Ligands

Nanopore‐Supported Metal Nanocatalysts for Efficient Hydrogen Generation from Liquid‐Phase Chemical Hydrogen Storage Materials

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Formic Acid‐Based Liquid Organic Hydrogen Carrier System with Heterogeneous Catalysts

Cited by 143 publications

References 123 publications

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Visible‐Light Photocatalytic Reduction of CO2 to Formic Acid with a Ru Catalyst Supported by N,N′‐Bis(diphenylphosphino)‐2,6‐diaminopyridine Ligands

Nanopore‐Supported Metal Nanocatalysts for Efficient Hydrogen Generation from Liquid‐Phase Chemical Hydrogen Storage Materials

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Visible‐Light Photocatalytic Reduction of CO₂ to Formic Acid with a Ru Catalyst Supported by N,N′‐Bis(diphenylphosphino)‐2,6‐diaminopyridine Ligands