Photoelectrochemical N-2-to-NH3 Fixation with High Efficiency and Rates via Optimized Si-Based System at Positive Potential versus Li0/+

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F23%3A10468479" target="_blank" >RIV/00216208:11320/23:10468479 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=uAwpScPDYb" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=uAwpScPDYb</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/adma.202211894" target="_blank" >10.1002/adma.202211894</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Photoelectrochemical N-2-to-NH3 Fixation with High Efficiency and Rates via Optimized Si-Based System at Positive Potential versus Li0/+

Popis výsledku v původním jazyce

As a widely used commodity chemical, ammonia is critical for producing nitrogen-containing fertilizers and serving as the promising zero-carbon energy carrier. Photoelectrochemical nitrogen reduction reaction (PEC NRR) can provide a solar-powered green and sustainable route for synthesis of ammonia (NH3). Herein, an optimum PEC system is reported with an Si-based hierarchically-structured PdCu/TiO2/Si photocathode and well-thought-out trifluoroethanol as the proton source for lithium-mediated PEC NRR, achieving a record high NH3 yield of 43.09 mu g cm(-2) h(-1) and an excellent faradaic efficiency of 46.15% under 0.12 MPa O-2 and 3.88 MPa N-2 at 0.07 V versus lithium(0/+) redox couple (vs Li0/+). PEC measurements coupled with operando characterization reveal that the PdCu/TiO2/Si photocathode under N-2 pressures facilitate the reduction of N-2 to form lithium nitride (Li3N), which reacts with active protons to produce NH3 while releasing the Li+ to reinitiate the cycle of the PEC NRR. The Li-mediated PEC NRR process is further enhanced by introducing small amount of O-2 or CO2 under pressure by accelerating the decomposition of Li3N. For the first time, this work provides mechanistic understanding of the lithium-mediated PEC NRR process and opens new avenues for efficient solar-powered green conversion of N-2-to-NH3.

Název v anglickém jazyce

Photoelectrochemical N-2-to-NH3 Fixation with High Efficiency and Rates via Optimized Si-Based System at Positive Potential versus Li0/+

Popis výsledku anglicky

As a widely used commodity chemical, ammonia is critical for producing nitrogen-containing fertilizers and serving as the promising zero-carbon energy carrier. Photoelectrochemical nitrogen reduction reaction (PEC NRR) can provide a solar-powered green and sustainable route for synthesis of ammonia (NH3). Herein, an optimum PEC system is reported with an Si-based hierarchically-structured PdCu/TiO2/Si photocathode and well-thought-out trifluoroethanol as the proton source for lithium-mediated PEC NRR, achieving a record high NH3 yield of 43.09 mu g cm(-2) h(-1) and an excellent faradaic efficiency of 46.15% under 0.12 MPa O-2 and 3.88 MPa N-2 at 0.07 V versus lithium(0/+) redox couple (vs Li0/+). PEC measurements coupled with operando characterization reveal that the PdCu/TiO2/Si photocathode under N-2 pressures facilitate the reduction of N-2 to form lithium nitride (Li3N), which reacts with active protons to produce NH3 while releasing the Li+ to reinitiate the cycle of the PEC NRR. The Li-mediated PEC NRR process is further enhanced by introducing small amount of O-2 or CO2 under pressure by accelerating the decomposition of Li3N. For the first time, this work provides mechanistic understanding of the lithium-mediated PEC NRR process and opens new avenues for efficient solar-powered green conversion of N-2-to-NH3.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10305 - Fluids and plasma physics (including surface physics)

Projekt

<a href="/cs/project/LM2023072" target="_blank" >LM2023072: Laboratoř fyziky povrchů – Vodíkové technologické centrum</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>S - Specificky vyzkum na vysokych skolach

Rok uplatnění

2023

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Advanced Materials

ISSN

0935-9648

e-ISSN

1521-4095

Svazek periodika

35

Číslo periodika v rámci svazku

21

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

9

Strana od-do

2211894

Kód UT WoS článku

000961615300001

EID výsledku v databázi Scopus

2-s2.0-85151954887