Influence of the proton relay spacer on hydrogen electrocatalysis by cobalt hangman porphyrins

Author(s):  
Manolis M. Roubelakis ◽  
D. Kwabena Bediako ◽  
Dilek K. Dogutan ◽  
Daniel G. Nocera
Keyword(s):  
2021 ◽  
Vol 50 (14) ◽  
pp. 4783-4788
Author(s):  
Jie Yang ◽  
Shuanglin He ◽  
Qianqian Wu ◽  
Ping Zhang ◽  
Lin Chen ◽  
...  

A bio-inspired manganese molecular catalyst featuring an intramolecular aniline as a proton relay was synthesized and used for hydrogen production. Electrochemical measurements with this complex show excellent activity (turnover frequency over 104 s−1).


2015 ◽  
Vol 51 (51) ◽  
pp. 10334-10336 ◽  
Author(s):  
Mohamed E. Moustafa ◽  
Paul D. Boyle ◽  
Richard J. Puddephatt

A phenol substituent has a dramatic effect on the oxidation of a dimethylplatinum(ii) complex with O2.


2013 ◽  
Vol 52 (51) ◽  
pp. 13518-13520 ◽  
Author(s):  
David Schilter ◽  
Thomas B. Rauchfuss
Keyword(s):  

2015 ◽  
Vol 1 (7) ◽  
pp. e1500263 ◽  
Author(s):  
Akihiko Nakamura ◽  
Takuya Ishida ◽  
Katsuhiro Kusaka ◽  
Taro Yamada ◽  
Shinya Fushinobu ◽  
...  

Hydrolysis of carbohydrates is a major bioreaction in nature, catalyzed by glycoside hydrolases (GHs). We used neutron diffraction and high-resolution x-ray diffraction analyses to investigate the hydrogen bond network in inverting cellulase PcCel45A, which is an endoglucanase belonging to subfamily C of GH family 45, isolated from the basidiomycete Phanerochaete chrysosporium. Examination of the enzyme and enzyme-ligand structures indicates a key role of multiple tautomerizations of asparagine residues and peptide bonds, which are finally connected to the other catalytic residue via typical side-chain hydrogen bonds, in forming the “Newton’s cradle”–like proton relay pathway of the catalytic cycle. Amide–imidic acid tautomerization of asparagine has not been taken into account in recent molecular dynamics simulations of not only cellulases but also general enzyme catalysis, and it may be necessary to reconsider our interpretation of many enzymatic reactions.


2003 ◽  
Vol 51 (2) ◽  
pp. 289-298 ◽  
Author(s):  
Assen Koumanov ◽  
Jordi Benach ◽  
Silvia Atrian ◽  
Roser Gonzàlez-Duarte ◽  
Andrey Karshikoff ◽  
...  

2014 ◽  
Vol 83 (2) ◽  
pp. 268-281 ◽  
Author(s):  
Rui Zhang ◽  
Anirban Bhattacharjee ◽  
Martin J. Field ◽  
Dennis R. Salahub

2019 ◽  
Vol 38 (6) ◽  
pp. 1391-1396 ◽  
Author(s):  
Neeraj Kumar ◽  
Jonathan M. Darmon ◽  
Charles J. Weiss ◽  
Monte L. Helm ◽  
Simone Raugei ◽  
...  

Materials ◽  
2018 ◽  
Vol 11 (7) ◽  
pp. 1202 ◽  
Author(s):  
Shuntaro Tsubaki ◽  
Shogo Hayakawa ◽  
Tadaharu Ueda ◽  
Tomohiko Mitani ◽  
Ei-ichi Suzuki ◽  
...  

Electromagnetic waves, such as microwaves, have been used to enhance various chemical reactions over polyoxometalates. The dielectric properties of catalysts are among the relevant parameters facilitating catalytic reactions under electromagnetic radiation. This study describes the dielectric properties of polyoxometalate catalysts in aqueous and organic solutions to understand the mechanism of interactions between polyoxometalates and electromagnetic waves. Specific loss factors of polyoxometalates were observed at lower frequencies (<1 GHz) by the ionic conduction of the polyoxometalate solution. The evolution of ionic conduction depended strongly on cations rather than anions. Proton-type polyoxometalates exhibited significantly higher loss factors than other cations did. The activation energy for ionic conduction in protonated silicotungstic acid (H4SiW12O40) was significantly low in water (7.6–14.1 kJ/mol); therefore, the high loss factor of protonated polyoxometalates in water was attributed to the proton relay mechanism (i.e., Grotthuss mechanism). The results suggested that the proton relay mechanism at the radio-frequency band is critical for generating selective interactions of polyoxometalates with applied electromagnetic fields.


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