Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and...Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and is therefore of great interest from an academic and industrial point of view. Very recently,novel metal-free mesoporous nitrogen-doped carbon catalysts have attracted large attention due to the unique reactivity and selectivity for the electrochemical hydrogen peroxide formation [1–3]. In this work,we provide deeper insights into the electrocatalytic activity, selectivity and durability of novel metal-free mesoporous nitrogen-doped carbon catalyst for the peroxide formation with a particular emphasis on the influence of experimental reaction parameters such as p H value and electrode potential for three different electrolytes. We used two independent approaches for the investigation of electrochemical hydrogen peroxide formation, namely rotating ring-disk electrode(RRDE) technique and photometric UV–VIS technique. Our electrochemical and photometric results clearly revealed a considerable peroxide formation activity as well as high catalyst durability for the metal-free nitrogen-doped carbon catalyst material in both acidic as well as neutral medium at the same electrode potential under ambient temperature and pressure. In addition, the obtained electrochemical reactivity and selectivity indicate that the mechanisms for the electrochemical formation and decomposition of peroxide are strongly dependent on the p H value and electrode potential.展开更多
Electrochemical production of hydrogen peroxide(H_(2)O_(2))via the two-electron(2e-)pathway of oxygen reduction reaction(ORR)supplies an auspicious alternative to the current industrial anthraquinone process.Nonethele...Electrochemical production of hydrogen peroxide(H_(2)O_(2))via the two-electron(2e-)pathway of oxygen reduction reaction(ORR)supplies an auspicious alternative to the current industrial anthraquinone process.Nonetheless,it still lacks efficient electrocatalysts to achieve high ORR activity together with 2e-selectivity simultaneously.Herein,a boron-doped defective nanocarbon(B-DC)electrocatalyst is synthesized by using fullerene frameworks as the precursor and boric oxide as the boron source.The obtained B-DC materials have a hierarchical porous structure,befitting boron dopants,and abundant topological pentagon defects,exhibiting a high ORR onset potential of 0.78 V and a dominated 2e-selectivity(over 95%).Remarkably,when B-DC electrocatalyst is employed in a real device,it achieves a high H_(2)O_(2) yield rate(247 mg·L^(-1)·h^(-1)),quantitative Faraday efficiency(~100%),and ultrafast organic pollutant degradation rate.The theoretical calculation reveals that the synergistic effect of topological pentagon defects and the incorporation of boron dopants promote the activation of the O_(2) molecule and facilitates the desorption of oxygen intermediate.This finding will be very helpful for the comprehension of the synergistic effect of topological defects and heteroatom dopants for boosting the electrocatalytic performance of nanocarbon toward H_(2)O_(2) production.展开更多
In this study,a non-enzymatic hydrogen peroxide sensor was successfully fabricated on the basis of copper sulfide nanoparticles/reduced graphene oxide(CuS/RGO) electrocatalyst.Using thiourea as reducing agent and su...In this study,a non-enzymatic hydrogen peroxide sensor was successfully fabricated on the basis of copper sulfide nanoparticles/reduced graphene oxide(CuS/RGO) electrocatalyst.Using thiourea as reducing agent and sulfur donor,CuS/RGO hybrid was synthesized through a facile one-pot hydrothermal method,where the reduction of GO and deposition of CuS nanoparticles on RGO occur simultaneously.The results confirmed that the CuS/RGO hybrid helps to prevent the aggregation of CuS nanoparticles.Electrochemical investigation showed that the as-prepared hydrogen peroxide sensor exhibited a low detection limit of 0.18μmol/L(S/N = 3),a good reproducibility(relative standard deviation(RSD) of4.21%),a wide linear range(from 3 to 1215 μmol/L) with a sensitivity of 216.9 μA L/mmol/cm-2 under the optimal conditions.Moreover,the as-prepared sensor also showed excellent selectivity and stability for hydrogen peroxide detection.The excellent performance of CuS/RGO hybrid,especially the lower detection limit than certain enzymes and noble metal nanomaterials ever reported,makes it a promising candidate for non-enzymatic H2O2 sensors.展开更多
基金supported by the Technische Universitat Berlin,the Max Planck Society and the Cluster of Excellence“Unifying Concepts in Catalysis(Uni Cat)”
文摘Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and is therefore of great interest from an academic and industrial point of view. Very recently,novel metal-free mesoporous nitrogen-doped carbon catalysts have attracted large attention due to the unique reactivity and selectivity for the electrochemical hydrogen peroxide formation [1–3]. In this work,we provide deeper insights into the electrocatalytic activity, selectivity and durability of novel metal-free mesoporous nitrogen-doped carbon catalyst for the peroxide formation with a particular emphasis on the influence of experimental reaction parameters such as p H value and electrode potential for three different electrolytes. We used two independent approaches for the investigation of electrochemical hydrogen peroxide formation, namely rotating ring-disk electrode(RRDE) technique and photometric UV–VIS technique. Our electrochemical and photometric results clearly revealed a considerable peroxide formation activity as well as high catalyst durability for the metal-free nitrogen-doped carbon catalyst material in both acidic as well as neutral medium at the same electrode potential under ambient temperature and pressure. In addition, the obtained electrochemical reactivity and selectivity indicate that the mechanisms for the electrochemical formation and decomposition of peroxide are strongly dependent on the p H value and electrode potential.
基金supported by the National Natural Science Foundation of China(Nos.22001084,21925104,and 92261204)Princess Nourah bint Abdulrahman University Researchers Supporting Project number(PNURSP2023R398)Princess Nourah bint Abdulrahman University,Riyadh,Saudi Arabia.
文摘Electrochemical production of hydrogen peroxide(H_(2)O_(2))via the two-electron(2e-)pathway of oxygen reduction reaction(ORR)supplies an auspicious alternative to the current industrial anthraquinone process.Nonetheless,it still lacks efficient electrocatalysts to achieve high ORR activity together with 2e-selectivity simultaneously.Herein,a boron-doped defective nanocarbon(B-DC)electrocatalyst is synthesized by using fullerene frameworks as the precursor and boric oxide as the boron source.The obtained B-DC materials have a hierarchical porous structure,befitting boron dopants,and abundant topological pentagon defects,exhibiting a high ORR onset potential of 0.78 V and a dominated 2e-selectivity(over 95%).Remarkably,when B-DC electrocatalyst is employed in a real device,it achieves a high H_(2)O_(2) yield rate(247 mg·L^(-1)·h^(-1)),quantitative Faraday efficiency(~100%),and ultrafast organic pollutant degradation rate.The theoretical calculation reveals that the synergistic effect of topological pentagon defects and the incorporation of boron dopants promote the activation of the O_(2) molecule and facilitates the desorption of oxygen intermediate.This finding will be very helpful for the comprehension of the synergistic effect of topological defects and heteroatom dopants for boosting the electrocatalytic performance of nanocarbon toward H_(2)O_(2) production.
基金received from the National Natural Science Foundation of China(Nos.21522606,21676246,21476201,21436007,U1462201,and 21376216)supported by Zhejiang Provincial Natural Science Foundation of China(No.LR17B060003)Major Science and Technology Project of Water Pollution Control and Management(No.2017ZX07101)
文摘In this study,a non-enzymatic hydrogen peroxide sensor was successfully fabricated on the basis of copper sulfide nanoparticles/reduced graphene oxide(CuS/RGO) electrocatalyst.Using thiourea as reducing agent and sulfur donor,CuS/RGO hybrid was synthesized through a facile one-pot hydrothermal method,where the reduction of GO and deposition of CuS nanoparticles on RGO occur simultaneously.The results confirmed that the CuS/RGO hybrid helps to prevent the aggregation of CuS nanoparticles.Electrochemical investigation showed that the as-prepared hydrogen peroxide sensor exhibited a low detection limit of 0.18μmol/L(S/N = 3),a good reproducibility(relative standard deviation(RSD) of4.21%),a wide linear range(from 3 to 1215 μmol/L) with a sensitivity of 216.9 μA L/mmol/cm-2 under the optimal conditions.Moreover,the as-prepared sensor also showed excellent selectivity and stability for hydrogen peroxide detection.The excellent performance of CuS/RGO hybrid,especially the lower detection limit than certain enzymes and noble metal nanomaterials ever reported,makes it a promising candidate for non-enzymatic H2O2 sensors.