Tandem Nitrogen Functionalization of Porous Carbon: Toward Immobilizing Highly Active Palladium Nanoclusters for Dehydrogenation of Formic Acid

Li, Zhangpeng; Yang, Xinchun; Tsumori, Nobuko; Liu, Zheng; Himeda, Yuichiro; Autrey, Tom; Xu, Qiang

doi:10.1021/acscatal.7b00053

Cited by 187 publications

(121 citation statements)

References 44 publications

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“…[75,76] However, MNPs are unstable on "naked" carbon because of the weak interactions between metal species and carbon surfaces, leading to low catalytic activities. [79] It was observed that the N-groups of the porous carbon could control the size and dispersion of the Pd nanoclusters. [77] An impressive TOF up to 2623 h −1 at 50 °C for FADH was achieved.…”

Section: Wwwadvancedsciencenewscommentioning

confidence: 99%

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Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Onishi

Iguchi

Yang

et al. 2018

Advanced Energy Materials

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128

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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%

“…Reproduced with permission [79]. Inset shows corresponding TOF values of the dehydrogenation of FA over the catalysts.…”

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confidence: 99%

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Onishi

Iguchi

Yang

et al. 2018

Advanced Energy Materials

Self Cite

128

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“…[1] However, the efficient production, release and controllable storage of hydrogen still remain challenging issues. Hydrogen (H 2 ) has been generally regarded as one of the propitious energy carriers to meet the growing demand for a clean and sustainable energy supply.…”

Section: Introductionmentioning

confidence: 99%

Nitrogen‐Decorated Porous Carbon Supported AgPd Nanoparticles for Boosting Hydrogen Generation from Formic Acid

Zhang

Shang

et al. 2018

Energy Tech

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Formic acid (FA) decomposition to yield molecular H2 is a promising approach in hydrogen economy. Design of selective, efficient catalysts for dehydrogenation of formic acid remains a challenging topic. Here, nitrogen‐doped porous carbon (NPC) nanosheets were fabricated with glucose as carbon source and g‐C3N4 as both the nitrogen source and self‐sacrificial template. Highly dispersed AgPd nanoparticles were supported on NPC successfully by a simple liquid impregnation approach. The optimized catalyst Ag1Pd9@NPC exhibits high catalytic activity (total turnover frequency up to 3000 h−1) and 100 % hydrogen selectivity for the dehydrogenation reaction of FA at 50 °C. Our study demonstrated that the synergistic effects between the nitrogen‐doped carbon nanosheets support and AgPd nanoparticles play a pivotal role for the efficient catalytic dehydrogenation of formic acid.

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“…When the growth rate is greater than the nucleation rate of PMNCs, this leads to the overgrowth of PMNCs, that is, nanocrystals with the larger sizes . To enhance the affinity between carbon supports and metal precursors/nanocrystals, doping carbon supports with heteroatoms (e.g., S and N) has been reported by Nazar, Xu, and our group . Heteroatom dopants show strong affinity to metal precursors/nanocrystals, which essentially anchor nanocrystals through metal−N and metal−S bindings.…”

Section: Figurementioning

confidence: 92%

Ultrafine and Ligand‐Free Precious Metal (Ru, Ag, Au, Rh and Pd) Nanoclusters Supported on Phosphorus‐Doped Carbon

Liu

Zhong

et al. 2018

Chemistry A European J

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We report the use of phosphorus-doped carbon (P-C) as support to grow ultrasmall (1-3 nm) and ligand-free precious metal nanocrystals (PMNCs) via chemical reduction. We show that the valence states of surface phosphorus species are critical in tuning the affinity between the carbon support and metal precursors, which rationally controls the loading size and uniformity of resultant PMNCs. Five kinds of PMNCs, including Ru, Ag, Au, Rh, and Pd, were grown in situ to demonstrate the key role of surface phosphorus sites on the P-C support. As a proof-of-concept application, Ru nanocatalysts with an average diameter of 1.0±0.2 nm supported on P-C were examined for the electrocatalytic hydrogen evolution reaction (HER). Ultrasmall and ligand-free Ru nanocatalysts exhibited superior HER activity and stability compared to its counterparts with surface agents or larger sizes. An overpotential of 27.6 mV (vs. reversible hydrogen electrode) for Ru nanocatalysts was achieved at a current density of 10 mA cm . This novel method opens a new avenue to immobilize ligand-free and well-dispersed PMNCs on carbon; and, more importantly, it provides a new library of supported PMNCs with high catalytic activity.

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Tandem Nitrogen Functionalization of Porous Carbon: Toward Immobilizing Highly Active Palladium Nanoclusters for Dehydrogenation of Formic Acid

Cited by 187 publications

References 44 publications

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Development of Effective Catalysts for Hydrogen Storage Technology Using Formic Acid

Nitrogen‐Decorated Porous Carbon Supported AgPd Nanoparticles for Boosting Hydrogen Generation from Formic Acid

Ultrafine and Ligand‐Free Precious Metal (Ru, Ag, Au, Rh and Pd) Nanoclusters Supported on Phosphorus‐Doped Carbon

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