TY - JOUR
T1 - Tandem electrocatalytic-catalytic conversion of nitrate and waste polylactic acid to alanine
AU - Teng, Xue
AU - Liang, Shaozhen
AU - Shi, Kai
AU - Chen, Lisong
AU - Shi, Jianlin
N1 - Publisher Copyright:
© 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences
PY - 2025/9
Y1 - 2025/9
N2 - Herein, a tandem electrocatalytic-catalytic method is employed to produce valuable alanine from nitrate and waste polylactic acid (PLA). Initially, two strategies are proposed to enhance the performance of electrocatalytic NO3− reduction reaction (NO3−RR): optimizing NO3− adsorption and accelerating water dissociation by modulating the cathode electrocatalyst. Fe-regulated Co nanosheets (Fe0.33-Co(OH)2 NSs) have been developed as an efficient electrocatalyst, which demonstrate a remarkable Faradaic efficiency (FE) of 98.2%, with a corresponding yield rate of 10.7 mg h−1 cm−2 for NO3−RR to NH3 at −0.1 V vs. RHE. Additionally, ∼95% FEs of NH3 at −200 mA cm−2 have been maintained for >430 h in the alkaline solution. Subsequently, in situ technologies have been utilized to elucidate the NO3−RR pathways, the structure transformation of the electrocatalysts, and the effects of Fe-induced work function reduction and electron enrichment at Co sites on electrocatalytic activity. Finally, alanine is synthesized by using PLA and the generated NH3 as the raw reactants on the Ru/TiO2 catalyst, achieving maximum yield and selectivity of 81.3% and 91.8%, respectively, which provides a novel approach to utilize the nitrogen resource and mitigate plastic pollution.
AB - Herein, a tandem electrocatalytic-catalytic method is employed to produce valuable alanine from nitrate and waste polylactic acid (PLA). Initially, two strategies are proposed to enhance the performance of electrocatalytic NO3− reduction reaction (NO3−RR): optimizing NO3− adsorption and accelerating water dissociation by modulating the cathode electrocatalyst. Fe-regulated Co nanosheets (Fe0.33-Co(OH)2 NSs) have been developed as an efficient electrocatalyst, which demonstrate a remarkable Faradaic efficiency (FE) of 98.2%, with a corresponding yield rate of 10.7 mg h−1 cm−2 for NO3−RR to NH3 at −0.1 V vs. RHE. Additionally, ∼95% FEs of NH3 at −200 mA cm−2 have been maintained for >430 h in the alkaline solution. Subsequently, in situ technologies have been utilized to elucidate the NO3−RR pathways, the structure transformation of the electrocatalysts, and the effects of Fe-induced work function reduction and electron enrichment at Co sites on electrocatalytic activity. Finally, alanine is synthesized by using PLA and the generated NH3 as the raw reactants on the Ru/TiO2 catalyst, achieving maximum yield and selectivity of 81.3% and 91.8%, respectively, which provides a novel approach to utilize the nitrogen resource and mitigate plastic pollution.
KW - Adsorption of NO
KW - Electrocatalytic NORR
KW - Fe-regulated Co(OH) nanosheets
KW - Hydrogenation of N-containing intermediates
KW - Tandem electrocatalytic-catalytic synthesis of alanine
UR - https://www.scopus.com/pages/publications/105005487744
U2 - 10.1016/j.jechem.2025.04.067
DO - 10.1016/j.jechem.2025.04.067
M3 - 文章
AN - SCOPUS:105005487744
SN - 2095-4956
VL - 108
SP - 694
EP - 702
JO - Journal of Energy Chemistry
JF - Journal of Energy Chemistry
ER -