Electrocatalytic hydrogenation of lignin monomer to methoxy-cyclohexanes with a high faradaic efficiency

2021 ◽  
Author(s):  
Miao Wang ◽  
Tao Peng ◽  
Chenxin Yang ◽  
Baiyao Liang ◽  
Henan Chen ◽  
...  
Keyword(s):  
Electrocatalytic Hydrogenation ◽  
Faradaic Efficiency ◽  
Commercial Interest ◽  
Chemical Manufacture

Developing efficient renewable electrocatalytic processes for chemical manufacture is of commercial interest, especially from the biomass-derived feedstock. Selective electrocatalytic hydrogenation (ECH) of biomass-derived lignin monomers to high-value oxygen-functional compounds is...

scholarly journals Synthesis of Valeric Acid by Selective Electrocatalytic Hydrogenation of Biomass-Derived Levulinic Acid

Catalysts ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 692
Author(s):  
Yan Du ◽  
Xiao Chen ◽  
Ji Qi ◽  
Pan Wang ◽  
Changhai Liang
Keyword(s):  
Levulinic Acid ◽  
Active Sites ◽  
Valeric Acid ◽  
Future Research ◽  
Adsorbed Hydrogen ◽  
Electrocatalytic Hydrogenation ◽  
Ambient Conditions ◽  
Metallic Lead ◽  
Faradaic Efficiency ◽  
Lead Electrode

The electrocatalytic hydrogenation (ECH) of biomass-derived levulinic acid (LA) is a promising strategy to synthetize fine chemicals under ambient conditions by replacing the thermocatalytic hydrogenation at high temperature and high pressure. Herein, various metallic electrodes were investigated in the ECH of LA in a H-type divided cell. The effects of potential, electrolyte concentration, reactant concentration, and temperature on catalytic performance and Faradaic efficiency were systematically explored. The high conversion of LA (93%) and excellent “apparent” selectivity to valeric acid (VA) (94%) with a Faradaic efficiency of 46% can be achieved over a metallic lead electrode in 0.5 M H2SO4 electrolyte containing 0.2 M LA at an applied voltage of −1.8 V (vs. Ag/AgCl) for 4 h. The combination of adsorbed LA and adsorbed hydrogen (Hads) on the surface of the metallic lead electrode is key to the formation of VA. Interestingly, the reaction performance did not change significantly after eight cycles, while the surface of the metallic lead cathode became rough, which may expose more active sites for the ECH of LA to VA. However, there was some degree of corrosion for the metallic lead cathode in this strong acid environment. Therefore, it is necessary to improve the leaching-resistance of the cathode for the ECH of LA in future research.

Isolated single-atom Pt sites for highly selective electrocatalytic hydrogenation of formaldehyde to methanol

2020 ◽  
Vol 8 (18) ◽  
pp. 8913-8919 ◽  
Author(s):  
Shunzheng Zhao ◽  
Yanfeng Wen ◽  
Xianyun Peng ◽  
Yuying Mi ◽  
Xijun Liu ◽  
...  
Keyword(s):  
Single Atom ◽  
High Yield ◽  
Electrocatalytic Hydrogenation ◽  
Electrochemical Hydrogenation ◽  
Faradaic Efficiency ◽  
Single Atoms ◽  
Yield Rate

Pt single atoms anchored on ultrathin Ti3C2Tx nanosheets can effectively catalyze the electrochemical hydrogenation of formaldehyde to methanol with a desirable faradaic efficiency of 95.8% and a record high yield rate of 30.7 mg h−1 mgcat.−1.

scholarly journals Electrocatalytic hydrogenation of guaiacol in diverse electrolytes using a slurry reactor

2019 ◽  
Author(s):  
Yanuar Philip Wijaya
Keyword(s):  
Reduction Process ◽  
Slurry Reactor ◽  
Catalyst Loading ◽  
Electrocatalytic Reduction ◽  
Electrocatalytic Hydrogenation ◽  
Perchloric Acid Solution ◽  
Faradaic Efficiency ◽  
Mild Conditions ◽  
Constant Potential ◽  
Low Catalyst Loading

Electrocatalytic hydrogenation-hydrogenolysis (ECH) of guaiacol was performed in an H-cell type of slurry reactor configuration with Pt/C catalyst. Different pairs of electrolytes, in catholyte-anolyte combinations, were investigated by constant potential chronocoulometry, showing that the acidic anolyte is preferable for an effective ECH. The advantages of this slurry reactor are mainly attributed to the enhanced Faradaic efficiency and recoverability of the catalyst. High guaiacol conversion (>90%) can be achieved at mild conditions (307 K, 1 atm) in perchloric acid solution (0.5 M), resulting in 54% cyclohexanol selectivity at moderate Faradaic efficiency (53%) and low catalyst loading. This work opens up the possibility of renewable synthesis of valuable chemicals from biomass-derived substrates via electrocatalytic reduction process at mild conditions.

scholarly journals Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Suheng Wang ◽  
Kelechi Uwakwe ◽  
Liang Yu ◽  
Jinyu Ye ◽  
Yuezhou Zhu ◽  
...  
Keyword(s):  
Ethylene Production ◽  
High Efficiency ◽  
Ambient Pressure ◽  
Industrial Process ◽  
Electrocatalytic Hydrogenation ◽  
Hydrogen Electrode ◽  
Faradaic Efficiency ◽  
Mild Conditions ◽  
Highly Efficient ◽  
Cu Catalyst

AbstractRenewable energy-based electrocatalytic hydrogenation of acetylene to ethylene (E-HAE) under mild conditions is an attractive substitution to the conventional energy-intensive industrial process, but is challenging due to its low Faradaic efficiency caused by competitive hydrogen evolution reaction. Herein, we report a highly efficient and selective E-HAE process at room temperature and ambient pressure over the Cu catalyst. A high Faradaic efficiency of 83.2% for ethylene with a current density of 29 mA cm−2 is reached at −0.6 V vs. the reversible hydrogen electrode. In-situ spectroscopic characterizations combined with first-principles calculations reveal that electron transfer from the Cu surface to adsorbed acetylene induces preferential adsorption and hydrogenation of the acetylene over hydrogen formation, thus enabling a highly selective E-HAE process through the electron-coupled proton transfer mechanism. This work presents a feasible route for high-efficiency ethylene production from E-HAE.

scholarly journals Selective electrocatalytic hydrogenation of bio-oil to oxygenated chemicals via suppression of deoxygenation

2021 ◽  
Author(s):  
Tao Peng ◽  
Taotao Zhuang ◽  
Yu Yan ◽  
Jin Qian ◽  
Graham Dick ◽  
...  
Keyword(s):  
Room Temperature ◽  
Ambient Pressure ◽  
Low Carbon ◽  
Electrocatalytic Hydrogenation ◽  
Faradaic Efficiency ◽  
Renewable Chemicals ◽  
Oxygenated Hydrocarbons ◽  
Bio Oil ◽  
Partial Current

Abstract Catalytic hydrogenation of bio-oil provides an avenue to produce renewable chemicals. To this end, electrocatalytic hydrogenation is especially interesting when powered using low-carbon electricity; however, it has to date lacked the needed selectivity: when hydrogenating bio-oil to oxygenated hydrocarbons, for example, it reduces the desired oxygenated groups (-OH and -OCH3). Here we report that Rh and Au modulate electronic structure of Pt and steer intermediate energetics to favor the hydrogenation while suppressing deoxygenation using computational studies and in-situ spectroscopies. PtRhAu catalysts achieve a record 47% faradaic efficiency (FE) and a partial current density (Jp) of 28 mA·cm-2 toward oxygenated 2-methoxycyclohexanol from lignin-derived guaiacol under room temperature and ambient pressure, representing 1.5x FE and 3.5x Jp increases compared to the best prior reports. We further demonstrate an integrated lignin biorefinery where wood-derived lignin oils are selectively hydrogenated and funneled to the oxygenated 2-methoxy-4-propylcyclohexanol using PtRhAu catalysts.

Nano-Folded Gold Electrocatalysts Enhance the Selectivity of Carbon Dioxide Reduction

2019 ◽  
Author(s):  
Kam Sang Kwok ◽  
Yuxuan Wang ◽  
Michael Cao ◽  
Hao Shen ◽  
Weinan Xu ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Mass Transport ◽  
Gold Film ◽  
X Ray Diffraction ◽  
Thin Gold Film ◽  
Faradaic Efficiency ◽  
X Ray ◽  
Transmission Electron ◽  
Carbon Monoxide Formation ◽  
Catalytic Interfaces

<p>The local structure and geometry of catalytic interfaces can influence the selectivity of chemical reactions. Here, using a pre-strained polymer, we uniaxially compress a thin gold film to form a nano-folded catalyst. We observe two kinds of folds and can tune the ratio of loose to tight folds by varying the extent of pre-strain in the polymer. We characterize the nano-folded catalysts using x-ray diffraction, scanning, and transmission electron microscopy. We observe grain reorientation and coarsening in the nano-folded gold catalysts. Electroreduction of carbon dioxide with these nano-folded catalysts reveals an enhancement of Faradaic efficiency for carbon monoxide formation by a factor of about four. This result suggests that electrolyte mass transport limitations and an increase of the local pH in the tight folds of the catalyst outweigh the effects of alterations in grain characteristics. Together, our studies demonstrate that nano-folded geometries can significantly alter grain characteristics, mass transport, and catalytic selectivity. </p>

Electrocatalytic hydrogenation of alkenes on LaNi5 electrodes

2000 ◽  
Vol 487 (1) ◽  
pp. 31-36 ◽  
Author(s):  
G.M.R van Druten ◽  
E Labbé ◽  
V Paul-Boncour ◽  
J Périchon ◽  
A Percheron-Guégan
Keyword(s):  
Electrocatalytic Hydrogenation

Optically and Electrocatalytically Decoupled Si Photocathodes with a Porous Carbon Nitride Catalyst for Nitrogen Reduction with Over 61.8% Faradaic Efficiency

2021 ◽  
pp. 2100812
Author(s):  
Karthik Peramaiah ◽  
Vinoth Ramalingam ◽  
Hui‐Chun Fu ◽  
Merfat M. Alsabban ◽  
Rafia Ahmad ◽  
...  
Keyword(s):  
Porous Carbon ◽  
Carbon Nitride ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction

Zr-doped α-FeOOH with High Faradaic Efficiency for Electrochemical Nitrogen Reduction Reaction

2021 ◽  
pp. 150801
Author(s):  
Jiabin Tan ◽  
Xiaobo H ◽  
Fengxiang Yin ◽  
Xin Liang ◽  
Guoru Li ◽  
...  
Keyword(s):  
Reduction Reaction ◽  
Faradaic Efficiency ◽  
Nitrogen Reduction

scholarly journals Insights on forming N,O-coordinated Cu single-atom catalysts for electrochemical reduction CO2 to methane

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yanming Cai ◽  
Jiaju Fu ◽  
Yang Zhou ◽  
Yu-Chung Chang ◽  
Qianhao Min ◽  
...  
Keyword(s):  
Energy Barrier ◽  
Active Sites ◽  
Theoretical Calculations ◽  
High Energy ◽  
Single Atom ◽  
Faradaic Efficiency ◽  
High Energy Barrier ◽  
Catalytic Sites ◽  
Electron Reduction ◽  
First Time

AbstractSingle-atom catalysts (SACs) are promising candidates to catalyze electrochemical CO2 reduction (ECR) due to maximized atomic utilization. However, products are usually limited to CO instead of hydrocarbons or oxygenates due to unfavorable high energy barrier for further electron transfer on synthesized single atom catalytic sites. Here we report a novel partial-carbonization strategy to modify the electronic structures of center atoms on SACs for lowering the overall endothermic energy of key intermediates. A carbon-dots-based SAC margined with unique CuN2O2 sites was synthesized for the first time. The introduction of oxygen ligands brings remarkably high Faradaic efficiency (78%) and selectivity (99% of ECR products) for electrochemical converting CO2 to CH4 with current density of 40 mA·cm-2 in aqueous electrolytes, surpassing most reported SACs which stop at two-electron reduction. Theoretical calculations further revealed that the high selectivity and activity on CuN2O2 active sites are due to the proper elevated CH4 and H2 energy barrier and fine-tuned electronic structure of Cu active sites.

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