Electrochemical conversion of CO({2|two}) into hydrocarbons and oxygenates is envisioned as a promising path towards closing the carbon cycle in {modern|contemporary|modern day} {technology|technologies}. To this day, {however|nevertheless|nonetheless|even so|on the other hand|having said that}, the reaction mechanisms towards the plethora of {products|goods|items|merchandise|solutions} are disputed, complicating the {search for|look for} novel catalyst {materials|supplies|components}. {In order to|To be able to|As a way to|In an effort to|So as to|So that you can} conclusively {identify|determine|recognize} the rate-limiting {steps|actions|measures|methods} in CO reduction on Cu, we analyzed the mechanisms {on the|around the} basis of {constant|continuous|continual} {potential|possible|prospective} DFT kinetics and experiments at a wide {range of|selection of|array of} pH values ({3|three} – 13). We {find|discover|locate|uncover|come across|obtain} that *CO dimerization is energetically favoured {as the|because the} {rate|price} limiting step towards multi-carbon {products|goods|items|merchandise|solutions}. This {finding|discovering|locating|obtaining|acquiring|getting} is {consistent|constant} with our experiments, {where|exactly where} the reaction {rate|price} is {nearly|almost|practically} unchanged on an SHE {potential|possible|prospective} scale, even {under|below|beneath} acidic {conditions|circumstances|situations}. For methane, {both|each} theory and experiments indicate a {change|alter|modify|adjust|transform} {in the|within the|inside the} rate-limiting step with electrolyte pH {from the|in the} {first|initial|very first|1st|initially} protonation step in acidic/neutral {conditions|circumstances|situations} to a later {one|1|a single|one particular} in alkaline {conditions|circumstances|situations}. We also show, {through|via|by means of|by way of} a detailed {analysis|evaluation} {of the|from the|in the|on the|with the|of your} microkinetics, that a surface {combination|mixture} of *CO and *H is inconsistent {with the|using the|with all the|together with the} measured {current|present|existing} densities and Tafel slopes. {Finally|Lastly|Ultimately}, we {discuss|talk about|go over} the implications of our understanding for future mechanistic {studies|research} and catalyst {design|style|design and style}. Buy2460255-78-9 Buy99116-11-7 PMID:23865629
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