scholarly journals Heterogeneous Fe3 single-cluster catalyst for ammonia synthesis via an associative mechanism

2018 ◽  
Vol 9 (1) ◽  
Author(s):  
Jin-Cheng Liu ◽  
Xue-Lu Ma ◽  
Yong Li ◽  
Yang-Gang Wang ◽  
Hai Xiao ◽  
...  
2016 ◽  
Vol 18 (13) ◽  
pp. 9161-9166 ◽  
Author(s):  
Seoin Back ◽  
Yousung Jung

The nitrogen reduction reaction (NRR) pathways involving various N–N dissociation steps are found to be comparable to the conventional associative mechanism. The competitive hydrogen adsorption and evolution is revealed to negatively affect the NRR for two reasons, an increase in NRR overpotentials as a function of partial H-coverages as well as a decreased number of active sites.


2021 ◽  
Vol 8 (11) ◽  
Author(s):  
Constantinos D. Zeinalipour-Yazdi ◽  
Justin S. J. Hargreaves ◽  
Said Laassiri ◽  
C. Richard A. Catlow

In this review, we present the recent progress in ammonia synthesis research using density functional theory (DFT) calculations on various industrial catalysts, metal nitrides and nano-cluster-supported catalysts. The mechanism of ammonia synthesis on the industrial Fe catalyst is generally accepted to be a dissociative mechanism . We have recently found, using DFT techniques, that on Co 3 Mo 3 N (111) surfaces, an associative mechanism in the synthesis of ammonia can offer a new low-energy pathway that was previously unknown. In particular, we have shown that metal nitrides that are also known to have high activity for ammonia synthesis can readily form nitrogen vacancies which can activate dinitrogen, thereby promoting the associative mechanism. These fundamental studies suggest that a promising route to the discovery of low-temperature ammonia synthesis catalysts will be to identify systems that proceed via the associative mechanism, which is closer to the nitrogen-fixation mechanism occurring in nitrogenases.


2021 ◽  
Vol 4 (11) ◽  
pp. 959-967
Author(s):  
Qianru Wang ◽  
Jaysree Pan ◽  
Jianping Guo ◽  
Heine Anton Hansen ◽  
Hua Xie ◽  
...  

2019 ◽  
Author(s):  
Katsutoshi Sato ◽  
Shin-ichiro Miyahara ◽  
Yuta Ogura ◽  
Kotoko Tsujimaru ◽  
Yuichiro Wada ◽  
...  

<p>To mitigate global problems related to energy and global warming, it is helpful to develop an ammonia synthesis process using catalysts that are highly active under mild conditions. Here we show that the ammonia synthesis activity of Ru/Ba/LaCeO<i><sub>x</sub></i> pre-reduced at 700 °C is the highest reported among oxide-supported Ru catalysts. Our results indicate that low crystalline oxygen-deficient composite oxides, which include Ba<sup>2+</sup>, Ce<sup>3+</sup> and La<sup>3+</sup>, with strong electron-donating ability, accumulate on Ru particles and thus promote N≡N bond cleavage, which is the rate determining step for ammonia synthesis.</p>


2019 ◽  
Author(s):  
Katsutoshi Sato ◽  
Shin-ichiro Miyahara ◽  
Yuta Ogura ◽  
Kotoko Tsujimaru ◽  
Yuichiro Wada ◽  
...  

<p>To mitigate global problems related to energy and global warming, it is helpful to develop an ammonia synthesis process using catalysts that are highly active under mild conditions. Here we show that the ammonia synthesis activity of Ru/Ba/LaCeO<i><sub>x</sub></i> pre-reduced at 700 °C is the highest reported among oxide-supported Ru catalysts. Our results indicate that low crystalline oxygen-deficient composite oxides, which include Ba<sup>2+</sup>, Ce<sup>3+</sup> and La<sup>3+</sup>, with strong electron-donating ability, accumulate on Ru particles and thus promote N≡N bond cleavage, which is the rate determining step for ammonia synthesis.</p>


2020 ◽  
Author(s):  
Deon T. Benton ◽  
David H. Rakison

The ability to reason about causal events in the world is fundamental to cognition. Despite the importance of this ability, little is known about how adults represent causal events, what structure or form those representations take, and what the mechanism is that underpins such representations. We report four experiments with adults that examine the perceptual basis on which adults represent four-object launching sequences (Experiments 1 and 2), whether adults representations reflect sensitivity to the causal, perceptual, or causal and perceptual relation among the objects that comprise such sequences (Experiment 3), and whether such representations extend beyond spatiotemporal contiguity to include other low-level stimulus features such as an object’s shape and color (Experiment 4). Based on these results of the four experiments, we argue that a domain-general associative mechanism, rather a modular, domain-specific, mechanism subserves adults’ representations of four-object launching sequences.


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