Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation

Xiong, Yu; Dong, Juncai; Huang, Zheng-Qing; Xin, Pingyu; Chen, Wenxing; Wang, Yu; Li, Zhi; Zhao, Jianmin; Wang, Xing; Zhuang, Zhongbin; Ye, Jinyu; Cao, Rui; Gu, Lin; Sun, Shi‐Gang; Zhuang, Lin; Chen, Xiaoqing; Ye, Hua; Chen, Chen; Peng, Qing; Chang, Chun‐Ran; Wang, Dingsheng; Li, Yadong

doi:10.1038/s41565-020-0665-x

Cited by 440 publications

(287 citation statements)

References 64 publications

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“…For carbon-based electrodes, the CV peaks are less easily discernable but similar peak shapes to Pt plates have been reported before. [21][22][23][24] The effect of oscillating potentials on the FA oxidation reaction on Pt plate electrodes has been investigated and we identified a frequency of 100 Hz at a duty cycle of 50% between OCP and 0.8 V to yield the largest FA oxidation enhancement ( Figure S4) in accordance to a previous study. 14 In the following, we further elucidated the transient current responses upon potential switches and we explored the capability of oscillating potentials in illuminating reaction kinetics.…”

Section: Catalyst Characterizationsupporting

confidence: 87%

Coverage-Dependent Formic Acid Oxidation Reaction Kinetics Determined by Oscillating Potentials

Hülsey¹,

Lim²,

Wong³

et al. 2020

Preprint

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We report a methodology based on applying oscillating potentials to various electrocatalytically active metal surfaces during the formic acid oxidation reaction. Moderate frequency oscillations (0.1 to 10 Hz) allow us to control the coverage of intermediates on the surface, thus enable quantifying the transient effects (on the time scale of up to 10−4 s) of coverage on the reaction rate. We determined different coverage-dependences of turnover frequencies for Pt metal plate and various carbon-supported metal nanoparticle catalysts (Pt/C, Pd/C and Rh/C). This method therefore constitutes a valuable and simple tool for the elucidation of adsorbate coverages on metal surfaces and their resulting catalytic performance. We also demonstrate that dynamic catalytic processes can be analyzed semi-quantitatively with this new approach allowing the design of catalytic processes under optimized conditions.<br>

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Section: Catalyst Characterizationsupporting

confidence: 87%

Coverage-Dependent Formic Acid Oxidation Reaction Kinetics Determined by Oscillating Potentials

Hülsey¹,

Lim²,

Wong³

et al. 2020

Preprint

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“…The presence of metallic Rh(0) was confirmed with XPS, which showed a binding energy at 307.3 eV ( Figure S1). [37,52,53] Nitrogen-doped carbon (NC) has been used as a support for single-atom catalysts with transition metals such as Co, [54][55][56] Mn, [54] Ni, [54] Fe, [54] Rh, [57] and Pd. [58] Supported Rh on nitrogendoped carbon (Rh/NC-HCl and Rh/NC-IWI) were prepared using a modified high-temperature thermal treatment as discussed in detail in the experimental section.…”

Section: Resultsmentioning

confidence: 99%

“…Rh/NC synthesis . Rhodium supported on nitrogen‐doped carbon (Rh/NC‐HCl) was prepared similar to a method reported previously [55,57,73] . Carbon Black Pearls 2000 from Cabot Corporation was used as the carbon support.…”

Section: Methodsmentioning

confidence: 99%

Oxidative Alkenylation of Arenes Using Supported Rh Materials: Evidence that Active Catalysts are Formed by Rh Leaching

et al. 2020

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This work focuses on the synthesis of supported Rh materials and study of their efficacy as pre‐catalysts for the oxidative alkenylation of arenes. Rhodium particles supported on silica (Rh/SiO2; ∼3.6 wt% Rh) and on nitrogen‐doped carbon (Rh/NC; ∼1.0 wt% Rh) are synthesized and tested. Heating mixtures of Rh/SiO2 or Rh/NC with benzene and ethylene or α‐olefins and CuX2 {X=OPiv (trimethylacetate) or OHex (2‐ethyl hexanoate)} to 150 °C results in the production of alkenyl arenes. When using Rh/SiO2 or Rh/NC as catalyst precursor, the conversion of benzene and propylene or toluene and 1‐pentene yields a ratio of anti‐Markovnikov to Markovnikov products that is nearly identical to the same ratios as the molecular catalyst precursor [Rh(μ‐OAc)(η2‐C2H4)2]2. These results and other observations are consistent with the formation of active catalysts by leaching of soluble Rh from the supported Rh materials.

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“…To date, there are a few MOF precursors that are regularly employed to make MOF-derived carbons, such as ZIF-8 and ZIF-67. [21][22][23][24] ZIFs, a subset of MOFs, are constructed by imidazole ligands having a relatively high density of N-based coordination sites. 25 However, ZIFs are predominately constructed by Zn and Co cations limiting the type of the metallic species that are subsequently incorporated into the carbons.…”

Section: Introductionmentioning

confidence: 99%

A metal–organic framework/polymer derived catalyst containing single-atom nickel species for electrocatalysis

Yang

Zhang

et al. 2020

Chem. Sci.

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Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation

Cited by 440 publications

References 64 publications

Coverage-Dependent Formic Acid Oxidation Reaction Kinetics Determined by Oscillating Potentials

Coverage-Dependent Formic Acid Oxidation Reaction Kinetics Determined by Oscillating Potentials

Oxidative Alkenylation of Arenes Using Supported Rh Materials: Evidence that Active Catalysts are Formed by Rh Leaching

A metal–organic framework/polymer derived catalyst containing single-atom nickel species for electrocatalysis

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