Developing electrocatalysts that exhibit both high activity and ammonia selectivity for nitrate reduction is a significant and demanding challenge,primarily due to the complex nature of the multiple-electron reduction...Developing electrocatalysts that exhibit both high activity and ammonia selectivity for nitrate reduction is a significant and demanding challenge,primarily due to the complex nature of the multiple-electron reduction process involved.An encouraging approach involves coupling highly active precious metals with transition metals to enhance catalytic performance through synergy.Here,we report a ruthenium-nickel alloy catalyst with nanosheets(Ru-Ni NSs)structure that achieves a remarkable ammonia Faradaic efficiency of approximately 95.93%,alongside a yield rate of up to 6.11 g·h^(−1)·cm^(−2).Moreover,the prepared Ru-Ni NSs exhibit exceptional stability during continuous nitrate reduction in a flow reactor for 100 h,maintaining a Faradaic efficiency of approximately 90%and an ammonia yield of 37.4 mg·L^(−1)·h^(−1)using 0.05 M nitrate alkaline electrolyte.Mechanistic studies reveal that the catalytic process follows a two-step pathway,in which HONO serves as a migration intermediate.The presence of a partially oxidized Ru(002)surface enhances the adsorption of nitrate and facilitates the release of the migration intermediate by adjusting the strength of the electrostatic and covalent interactions between the adsorbate and the surface,respectively.On the other hand,the Ni(111)surface promotes the utilization of the migration intermediate and requires less energy for NH_(3)desorption.This tandem process contributes to a high catalytic activity of Ru-Ni NSs towards nitrate reduction.展开更多
The unsatisfactory nutrient slow-release and water-retention performance of traditional biochar-based compound fertilizers(BCF)severely limit their practical application.Herein,a new type of slow-release fertilizer wi...The unsatisfactory nutrient slow-release and water-retention performance of traditional biochar-based compound fertilizers(BCF)severely limit their practical application.Herein,a new type of slow-release fertilizer with high water retention was fabricated via the incorporation of hydrotalcite and starch into BCF,named as HS-BCF.The waterretention and nutrient releasing performance of the prepared HS-BCF and related nutrient slow-release mechanism were investigated.The results showed that the incorporation of hydrotalcite and starch into BCF could increase the soil water-retention ratio by 5-10%points.The accumulated N,P,and K leaching amounts of HS-BCF in soil within 30 days were 49.4%,13.3%,and 87.4%of BCF at most,respectively.Kinetic analysis indicated that the release of nutrients from HS-BCF was attributed to the coupling of the diffusion-controlled and relaxation-controlled mechanism.Moreover,hydrotalcite could bind with P in HS-BCF,contributing to the enhanced durability of P in HS-BCF.Finally,pot experiments showed that the N-P-K utilization efficiencies of HS-BCF were all higher than those of BCF due to a better synchronization between the nutrient release of HS-BCF and the uptake of tomato plants.Overall,the study may provide a promising strategy for simultaneously improving the water-retention and slow-release performance of traditional biochar-based fertilizers.展开更多
基金the National Natural Science Foundation of China(No.22006018)the General Project of Zhejiang Provincial Department of Education(No.Y202250180)+2 种基金the key Research and Development Project of Science and Technology Department of Zhejiang Province(No.2023C02019)the National Key Research and Development Program of China(No.2022YFE0127800)the Talent Startingup Project of Research Development Fund of Zhejiang A&F University(No.2034020103).
文摘Developing electrocatalysts that exhibit both high activity and ammonia selectivity for nitrate reduction is a significant and demanding challenge,primarily due to the complex nature of the multiple-electron reduction process involved.An encouraging approach involves coupling highly active precious metals with transition metals to enhance catalytic performance through synergy.Here,we report a ruthenium-nickel alloy catalyst with nanosheets(Ru-Ni NSs)structure that achieves a remarkable ammonia Faradaic efficiency of approximately 95.93%,alongside a yield rate of up to 6.11 g·h^(−1)·cm^(−2).Moreover,the prepared Ru-Ni NSs exhibit exceptional stability during continuous nitrate reduction in a flow reactor for 100 h,maintaining a Faradaic efficiency of approximately 90%and an ammonia yield of 37.4 mg·L^(−1)·h^(−1)using 0.05 M nitrate alkaline electrolyte.Mechanistic studies reveal that the catalytic process follows a two-step pathway,in which HONO serves as a migration intermediate.The presence of a partially oxidized Ru(002)surface enhances the adsorption of nitrate and facilitates the release of the migration intermediate by adjusting the strength of the electrostatic and covalent interactions between the adsorbate and the surface,respectively.On the other hand,the Ni(111)surface promotes the utilization of the migration intermediate and requires less energy for NH_(3)desorption.This tandem process contributes to a high catalytic activity of Ru-Ni NSs towards nitrate reduction.
基金Key Research and Development Project of Science and Technology Department of Zhejiang Province(2023C02019)National Key Research and Development Program of China(2022YFE0127800)+2 种基金National Natural Science Foundation of China(22006018)talent starting-up project of research development fund of Zhejiang A&F University(2034020103)Overseas Expertise Introduction Project for Discipline Innovation(111 Project D18008).
文摘The unsatisfactory nutrient slow-release and water-retention performance of traditional biochar-based compound fertilizers(BCF)severely limit their practical application.Herein,a new type of slow-release fertilizer with high water retention was fabricated via the incorporation of hydrotalcite and starch into BCF,named as HS-BCF.The waterretention and nutrient releasing performance of the prepared HS-BCF and related nutrient slow-release mechanism were investigated.The results showed that the incorporation of hydrotalcite and starch into BCF could increase the soil water-retention ratio by 5-10%points.The accumulated N,P,and K leaching amounts of HS-BCF in soil within 30 days were 49.4%,13.3%,and 87.4%of BCF at most,respectively.Kinetic analysis indicated that the release of nutrients from HS-BCF was attributed to the coupling of the diffusion-controlled and relaxation-controlled mechanism.Moreover,hydrotalcite could bind with P in HS-BCF,contributing to the enhanced durability of P in HS-BCF.Finally,pot experiments showed that the N-P-K utilization efficiencies of HS-BCF were all higher than those of BCF due to a better synchronization between the nutrient release of HS-BCF and the uptake of tomato plants.Overall,the study may provide a promising strategy for simultaneously improving the water-retention and slow-release performance of traditional biochar-based fertilizers.