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 electrocatalyti...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 NO_(3)^(-)reduction reaction(NO_(3)^(-)RR):optimizing NO_(3)^(-)adsorption and accelerating water dissociation by modulating the cathode electrocatalyst.Fe-regulated Co nanosheets(Fe_(0.33)-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 NO_(3)RR to NH_(3)at-0.1 V vs.RHE.Additionally,~95%FEs of NH_(3)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 NO_(3)^(-)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 NH_(3)as the raw reactants on the Ru/TiO_(2)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.展开更多
基金supported by the National Key R&D Program of China(2022YFB4002700)the National Natural Science Foundation of China(22475071)the Shanghai Science and Technology Committee Rising-Star Program(22QA1403400)。
文摘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 NO_(3)^(-)reduction reaction(NO_(3)^(-)RR):optimizing NO_(3)^(-)adsorption and accelerating water dissociation by modulating the cathode electrocatalyst.Fe-regulated Co nanosheets(Fe_(0.33)-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 NO_(3)RR to NH_(3)at-0.1 V vs.RHE.Additionally,~95%FEs of NH_(3)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 NO_(3)^(-)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 NH_(3)as the raw reactants on the Ru/TiO_(2)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.
