molecular catalyst
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Author(s):  
Jan Bühler ◽  
Jonas Zurflüh ◽  
Sebastian Siol ◽  
Olivier Blacque ◽  
Laurent Sévery ◽  
...  

Efficient catalytic oxidative C–H activation of organic substrates remains an important challenge in synthetic chemistry. Here, we show that the combination of a transition metal catalyst, surface immobilisation and an...


2022 ◽  
Author(s):  
Kento Kosugi ◽  
Hina Kashima ◽  
Mio Kondo ◽  
Shigeyuki Masaoka

We report a highly active copper-based catalyst for electrochemical CO2 reduction. Electrochemical analysis revealed that the maximum turnover frequency for CO2 to CO conversion reached to 1,460,000 s-1 at an...


2021 ◽  
Author(s):  
Lin Li ◽  
Biswanath Das ◽  
Ahibur Rahaman ◽  
Andrey Shatskiy ◽  
Fei Ye ◽  
...  

Electrochemical water splitting constitutes one of the most promising strategies for converting water into hydrogen-based fuels, and this technology is predicted to play a key role in our transition towards a carbon-neutral energy economy. To enable the design of cost-effective electrolysis cells based on this technology, new and more efficient anodes with augmented water splitting activity and stability will be required. Herein, we report an active molecular Ru-based catalyst for electrochemically-driven water oxidation and two simple methods for preparing anodes by attaching this catalyst onto multi-walled carbon nanotubes. The anodes modified with the molecular catalyst were characterized by a broad toolbox of microscopy and spectroscope techniques, and interestingly no RuO2 formation was detected during electrocatalysis over 4 h. These results demonstrate that the herein presented strategy can be used to prepare anodes that rival the performance of state-of-the-art metal oxide anodes.


2021 ◽  
Author(s):  
Jonas Peters ◽  
Pablo Garrido-Barros ◽  
Joseph Derosa ◽  
Matthew Chalkley

Abstract New electrochemical ammonia (NH3) synthesis technologies are of interest as a complementary route to the Haber-Bosch (HB) process for distributed fertilizer generation, and towards exploiting ammonia as a zero-carbon fuel produced via renewably-sourced electricity.1–4 Apropos of these goals is a surge of fundamental research targeting heterogeneous materials5–7 as electrocatalysts for the nitrogen reduction reaction (N2RR). These systems generally suffer from poor stability and NH3 selectivity; competitive hydrogen evolution reaction (HER) outcompetes N2RR.8 Molecular catalyst systems can be exquisitely tuned and offer an alternative strategy,9 but progress has thus far been thwarted by the same selectivity issue; HER dominates. Herein we describe a tandem catalysis strategy that offers a solution to this puzzle. A molecular complex that can mediate an N2 reduction cycle is partnered with a co-catalyst that interfaces the electrode and an acid to mediate concerted proton-electron transfer (CPET) steps, facilitating N−H bond formation at a favorable applied potential and overall thermodynamic efficiency. Without CPET, certain intermediates of the N2RR cycle would be unreactive via independent electron transfer (ET) or proton transfer (PT) steps, thereby shunting the system. Promisingly, complexes featuring several metals (W, Mo, Os, Fe) achieve N2RR electrocatalysis at the same applied potential in the presence of the CPET mediator, pointing to the generality of this tandem approach.


Author(s):  
Conor L. Rooney ◽  
Yueshen Wu ◽  
Zixu Tao ◽  
Hailiang Wang
Keyword(s):  

Small ◽  
2021 ◽  
Vol 17 (46) ◽  
pp. 2170243
Author(s):  
Satyanarayana Samireddi ◽  
V. Aishwarya ◽  
Indrajit Shown ◽  
Saravanakumar Muthusamy ◽  
Sreekuttan M. Unni ◽  
...  

2021 ◽  
Vol MA2021-02 (53) ◽  
pp. 1558-1558
Author(s):  
Matthew Liu ◽  
Dean Miller ◽  
William Abraham Tarpeh

Small ◽  
2021 ◽  
pp. 2103823
Author(s):  
Satyanarayana Samireddi ◽  
V. Aishwarya ◽  
Indrajit Shown ◽  
Saravanakumar Muthusamy ◽  
Sreekuttan M. Unni ◽  
...  

2021 ◽  
Author(s):  
Pablo Garrido-Barros ◽  
Joseph Derosa ◽  
Matthew Chalkley ◽  
Jonas Peters

New electrochemical ammonia (NH3) synthesis technologies are of interest as a complementary route to the Haber-Bosch (HB) process for distributed fertilizer generation, and towards exploiting ammonia as a zero-carbon fuel produced via renewably-sourced electricity. Apropos of these goals is a surge of fundamental research targeting heterogeneous materials as electrocatalysts for the nitrogen reduction reaction (N2RR). These systems generally suffer from poor stability and NH3 selectivity; competitive hydrogen evolution reaction (HER) outcompetes N2RR. Molecular catalyst systems can be exquisitely tuned and offer an alternative strategy, but progress has thus far been thwarted by the same selectivity issue; HER dominates. Herein we describe a tandem catalysis strategy that offers a solution to this puzzle. A molecular complex that can mediate an N2 reduction cycle is partnered with a co-catalyst that interfaces the electrode and an acid to mediate concerted proton-electron transfer (CPET) steps, facilitating N−H bond formation at a favorable applied potential and overall thermodynamic efficiency. Without CPET, certain intermediates of the N2RR cycle would be unreactive via independent electron transfer (ET) or proton transfer (PT) steps, thereby shunting the system. Promisingly, complexes featuring several metals (W, Mo, Os, Fe) achieve N2RR electrocatalysis at the same applied potential in the presence of the CPET mediator, pointing to the generality of this tandem approach.


2021 ◽  
Author(s):  
Francesca Arcudi ◽  
Luka Dordevik ◽  
Neil Schweitzer ◽  
Samuel Stupp ◽  
Emily Weiss

Abstract The production of polymer-grade ethylene requires the purification of ethylene feed from acetylene contaminant. Accomplishing this task by state-of-the-art thermal hydrogenation requires high temperature, external feed of H2 gas, and noble metal catalysts, and is not only expensive and energy-intensive but also prone to overhydrogenate to ethane. We report a photocatalytic system to reduce acetylene to ethylene with >99% selectivity for ethylene under both non-competitive (no ethylene co-feed) and competitive (ethylene co-feed) conditions, and near 100% conversion under the latter industrially relevant condition. Our system uses a molecular catalyst based on earth-abundant cobalt operating under ambient conditions and sensitized by either [Ru(bpy)3]2+ or an inexpensive organic semiconductor (mpg-CN) under visible light. These features and the use of water as a proton source offer substantial advantages over current hydrogenation technologies with respect to selectivity and sustainability.


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