Alkenols are important intermediates for the industrial manufacture of various commodities and fine chemicals.At present,alkenols are produced via thermocatalytic semihydrogenation of corresponding alkynols using prec...Alkenols are important intermediates for the industrial manufacture of various commodities and fine chemicals.At present,alkenols are produced via thermocatalytic semihydrogenation of corresponding alkynols using precious metal Pd-based catalysts in pressurized hydrogen atmosphere.In this work,we highlight an efficient electrocatalytic strategy for selectively reducing alkynols to alkenols under ambient conditions.Using 2-methyl-3-butyn-2-ol as a model alkynol,Cu3P nanoarrays anchored on Cu foam remarkably deliver an industrial-level partial current density of 0.79 A·cm^(-2) and a specific selectivity of 98%for 2-methyl-3-buten-2-ol in acidic solution.Over a 40-runs stability test,Cu3P nanoarrays maintain 90%alkynol conversion and 90%alkenol selectivity.Even in a large two-electrode flow electrolyser,the single-pass alkynol conversion and alkenol selectivity of Cu3P nanoarrays exceed 90%.Moreover,this selective electrocatalytic hydrogenation approach is broadly feasible for the production of various water-soluble alkenols.Electrochemical analyses,theoretical simulation and electrochemical in-situ infrared investigations together reveal that exothermic alkynol hydrogenation,facile alkenol desorption and formation of active H on Cu3P surfaces account for the excellent electrocatalytic performance.展开更多
基金financially supported by the National Natural Science Foundation of China(22005245 and 22201232)the Key Research and Development Program of Shaanxi Province(2023-YBGY-284)+3 种基金the Fundamental Research Funds for the Central Universities(G2022KY0606 and G2022KY05114)the Synergy Innovation Foundation of the University and Enterprise for Graduate Students in Northwestern Polytechnical University(CX2021037 and CX2022074)the Fundamental Research Funds for China Postdoctoral Science Foundation(BX2021247 and 2021M692635)the Natural Science Foundation of Shaanxi Province(2022JQ-083).
文摘Alkenols are important intermediates for the industrial manufacture of various commodities and fine chemicals.At present,alkenols are produced via thermocatalytic semihydrogenation of corresponding alkynols using precious metal Pd-based catalysts in pressurized hydrogen atmosphere.In this work,we highlight an efficient electrocatalytic strategy for selectively reducing alkynols to alkenols under ambient conditions.Using 2-methyl-3-butyn-2-ol as a model alkynol,Cu3P nanoarrays anchored on Cu foam remarkably deliver an industrial-level partial current density of 0.79 A·cm^(-2) and a specific selectivity of 98%for 2-methyl-3-buten-2-ol in acidic solution.Over a 40-runs stability test,Cu3P nanoarrays maintain 90%alkynol conversion and 90%alkenol selectivity.Even in a large two-electrode flow electrolyser,the single-pass alkynol conversion and alkenol selectivity of Cu3P nanoarrays exceed 90%.Moreover,this selective electrocatalytic hydrogenation approach is broadly feasible for the production of various water-soluble alkenols.Electrochemical analyses,theoretical simulation and electrochemical in-situ infrared investigations together reveal that exothermic alkynol hydrogenation,facile alkenol desorption and formation of active H on Cu3P surfaces account for the excellent electrocatalytic performance.
