Ultrahigh Electrocatalytic Conversion of Methane at Room Temperature

Ma, Ming; Jin, Bing; Li, Ping; Jung, Myung Sun; Kim, Sang Hyun; Cho, Yoonjun; Kim, Sungsoon; Moon, Jun Hyuk; Park, Jae Hyung

doi:10.1002/advs.201700379

Cited by 90 publications

(79 citation statements)

References 38 publications

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“…The high-energy MO sites are difficult to form thermochemically using O 2 (i.e., high G f ), but they can be generated by applying an anodic potential. [29] Ni(OH) 2 , [112] NiO/ ZrO 2 , [113,114] and Co 2 O 3 /ZrO 2 [115] have been explored as anode catalysts for methane activation at room temperature in carbonate electrolyte. The generation of methanol and higher alcohols such as propanol was observed by 1 H NMR or MS, but the TOF, TON, and Faradic efficiency were not qualified possibly due to the low yield.…”

Section: Electrocatalysts That Undergo Dehydrogenation Mechanismmentioning

confidence: 99%

Conversion of Methane into Liquid Fuels—Bridging Thermal Catalysis with Electrocatalysis

Yuan

Peng

et al. 2020

Advanced Energy Materials

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The direct partial oxidation of methane to methanol promises an energy‐efficient and environmental‐friendly utilization of natural gas. Unfortunately, current technologies confront a grand challenge in catalysis, particularly in the context of distributed sources. Research has been focused on the design of homogenous and heterogenous catalysts to improve the activation of methane under thermal and electrochemical conditions. However, the intrinsic relationship between thermal and electrochemical systems has not been exploited yet. This review intends to bridge the studies of thermal and electrochemical catalysts, in both homogenous and heterogenous systems, for methane activation from a mechanistic point of view. It is expected to provide a framework to rationalize the design of electrocatalysts beyond the state of art. First, methane activation systems reported previously are reviewed and classified into two basic mechanisms: dehydrogenation and deprotonation. Based on the mechanism types, activity and selectivity descriptors are defined to understand the performance of current catalysts and guide the design of future catalysts. Moreover, methods to enhance the activity and selectivity are discussed to emphasize the unique advantage of electrocatalysis in overcoming the limitations of traditional thermal catalysis. Finally, immense opportunities and challenges for catalyst design are discussed by unifying thermal and electrochemical catalysis.

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Section: Electrocatalysts That Undergo Dehydrogenation Mechanismmentioning

confidence: 99%

Conversion of Methane into Liquid Fuels—Bridging Thermal Catalysis with Electrocatalysis

Yuan

Peng

et al. 2020

Advanced Energy Materials

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“…MeOH, HCHO, HCOOH Radical [108] NiO Radical [111] Pt/C, Pt/C-ATO, Pd/C, Pd/C-ATO incorporation of V 2 O 5 into TiO 2 /RuO 2 /PTFE GDE suppressed the formation of formaldehyde and formic acid, thereby increased MeOH selectivity. [108] A 5.6 wt% V 2 O 5 loading to the GDE increased the current efficiency of the electrode to 57% at 2.0 V versus SCE.…”

Section: Electrochemical Systems For Ch 4 Oxidationmentioning

confidence: 99%

“…It is interesting to note that, unlike OH − ions, CO 3 2− ions donate oxygen ions with successive release of CO 2 , which generated a large change in the enthalpy of reaction, favoring oxidation kinetics even at low temperatures. [111] Additionally, the presence of the redox couple Ni 2+ /Ni 3+ (by the reaction, Ni(OH) 2 + OH − ↔ NiOOH + H 2 O + e − ) at 0.5-0.6 V vs SCE favored the oxidation process. The products were identified as different oxygenates, such as methanol, ethanol, isopropanol, formaldehyde, formate, acetate, acetone, and carbon monoxide.…”

Section: Electrolyte Mediated Ch 4 Oxidationmentioning

confidence: 99%

“…Following the idea of Spinner, Park's group recently designed ZrO 2 /Co 3 O 4 composite catalysts for the electrochemical oxidation of CH 4 at room temperature. [111] A series of composite catalysts were synthesized with different ratios of Co 3 O 4 and ZrO 2 . Electron microscopy ( Figure 7) images revealed that oval-shaped and uniform ZrO 2 nanoparticles were anchored on the surface of Co 3 O 4 nanoplates to make heterojunctions.…”

Section: Electrolyte Mediated Ch 4 Oxidationmentioning

confidence: 99%

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Catalytic Oxidation of Methane to Oxygenated Products: Recent Advancements and Prospects for Electrocatalytic and Photocatalytic Conversion at Low Temperatures

et al. 2020

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Methane is an important fossil fuel and widely available on the earth's crust. It is a greenhouse gas that has more severe warming effect than CO 2. Unfortunately, the emission of methane into the atmosphere has long been ignored and considered as a trivial matter. Therefore, emphatic effort must be put into decreasing the concentration of methane in the atmosphere of the earth. At the same time, the conversion of less valuable methane into value-added chemicals is of significant importance in the chemical and pharmaceutical industries. Although, the transformation of methane to valuable chemicals and fuels is considered the "holy grail," the low intrinsic reactivity of its C-H bonds is still a major challenge. This review discusses the advancements in the electrocatalytic and photocatalytic oxidation of methane at low temperatures with products containing oxygen atom(s). Additionally, the future research direction is noted that may be adopted for methane oxidation via electrocatalysis and photocatalysis at low temperatures.

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“…In this regard, Ma et al have reported that the electrochemical oxidation of methane in an electrolyzer can be used to produce higher alcohols such as propanol at room temperature. 14 Despite the demonstration of electrochemical oxidation of methane to methanol in previous reports, lack of consistency in the testing conditions and electrolytes used among the reports presents an additional challenge. A systematic study of the dependence of product distribution on applied potential, current, temperature, and pressure could facilitate the understanding of how various parameters affect the kinetics for methanol formation and aid in the advancement of this field.…”

Section: Challenges and Opportunitiesmentioning

confidence: 99%

Electrochemical Direct Partial Oxidation of Methane to Methanol

Jang

Shen

Morales‐Guio

2019

Joule

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Joonbaek Jang received his B.S. from Korea University in 2016. He then moved to the University of Pennsylvania where he obtained his M.S. working with Prof. Raymond J. Gorte. During his master's degree, Joonbaek used atomic layer deposition to modify metal oxide catalysts for the improvement of industrial catalytic processes. In 2018, he joined the Morales-Guio Lab in the Department of Chemical and Biomolecular Engineering at UCLA. Joonbaek is currently working toward the understanding of electrode/ electrolyte interfaces and mass transport effects in electrocatalytic processes for sustainable energy applications. Kangze Shen received his B.S. in Materials Chemistry from University of Science and Technology of China in 2018. His undergraduate research with Prof. Yitai Qian focused on the development of high-performance electrode materials for rechargeable Li-ion and Na-ion batteries. He then joined the Morales-Guio Lab in the Department of Chemical and Biomolecular Engineering at UCLA where he is working toward the understanding of electrocatalytic processes and electrochemical systems engineering in sustainable energy applications. Carlos G. Morales-Guio is an Assistant Professor of Chemical and Biomolecular Engineering at UCLA. The Morales-Guio Lab is interested in electrochemical catalysis, particularly with respect to energy and chemical transformations for sustainable energy applications. The lab is currently focused on understanding fundamentals of mass and charge transport coupled to electrochemical transformations that will guide the scale up of electrocatalytic reactors. Carlos received his B. Eng. degree from Osaka University in 2011 and his M.S. and Ph.D. in Chemistry and Chemical Engineering from EPFL in 2013 and 2016, respectively. Most recently, he was a postdoctoral research fellow at Stanford University before joining UCLA in 2018.

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Ultrahigh Electrocatalytic Conversion of Methane at Room Temperature

Cited by 90 publications

References 38 publications

Conversion of Methane into Liquid Fuels—Bridging Thermal Catalysis with Electrocatalysis

Conversion of Methane into Liquid Fuels—Bridging Thermal Catalysis with Electrocatalysis

Catalytic Oxidation of Methane to Oxygenated Products: Recent Advancements and Prospects for Electrocatalytic and Photocatalytic Conversion at Low Temperatures

Electrochemical Direct Partial Oxidation of Methane to Methanol

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