Nitrate synthesis is an important process for agriculture and industry,but suffers from energy-intensive steps including the synthesis and subsequent oxidation of ammonia.Herein,we present a selective N_(2)transformat...Nitrate synthesis is an important process for agriculture and industry,but suffers from energy-intensive steps including the synthesis and subsequent oxidation of ammonia.Herein,we present a selective N_(2)transformation to nitrate by guiding the charge neutralization of self-electrified water microdroplets in an artificial cloud generated with the portable ultrasonic atomizer.The electron and ion transfer in the charge neutralization of water microdroplets on metal micromesh enables an up to~40-fold increase in the reactivity of nitrate formation reaction driven by ultrasonic energy.A robust semi-continuous N_(2)oxidation by a Ni-mesh-screened cloud system was achieved,providing nitrate with~12 mM concentration every 20 h.These findings emphasize the potential of harnessing the microdroplet-mediated cloud electrochemistry of N_(2)in decentralizing the current mass production of fertilizer.展开更多
The purity of electronic-grade chemicals significantly impacts electronic components.Although crystallization has been used to purify cerium ammonium nitrate(CAN),the impurity removal mechanism underlying different cr...The purity of electronic-grade chemicals significantly impacts electronic components.Although crystallization has been used to purify cerium ammonium nitrate(CAN),the impurity removal mechanism underlying different crystallization parameters remains unclear.Traditional analytical methods of inductively coupled plasma mass spectrometry(ICP-MS)have problems in detecting trace Fe accurately,because of the high concentration of Ce and interference of polyatomic ions.Therefore,this study developed a new method integrating the standard addition and internal standard methods and explored the role of the kinetic energy discrimination mode.This new approach effectively overcomes Ce-related matrix interference and fills the gap in ultra-trace impurity detection.Furthermore,the study investigated the effects of cooling rate,seed mass loading and seed size on the removal of Fe impurity.The seed mass loading affects the average crystal size through regulating secondary nucleation and crystal growth.The removal of Fe in CAN is determined by surface adsorption and agglomeration.Under the condition of the cooling rate of 0.2 K·min^(-1),and addition of 0.5%(mass)600-680 μm seeds,the Fe content is the lowest,at only 0.24 mg·L^(-1),and the Fe removal rate reaches 92.28%.展开更多
基金supported by the National Key R&D Program of China(2022YFA1504603)the National Natural Science Foundation of China(22025206,22172163)+1 种基金the Dalian Innovation Support Plan for High Level Talents(2022RG13)the Fundamental Research Funds for the Central Universities(20720220008)。
文摘Nitrate synthesis is an important process for agriculture and industry,but suffers from energy-intensive steps including the synthesis and subsequent oxidation of ammonia.Herein,we present a selective N_(2)transformation to nitrate by guiding the charge neutralization of self-electrified water microdroplets in an artificial cloud generated with the portable ultrasonic atomizer.The electron and ion transfer in the charge neutralization of water microdroplets on metal micromesh enables an up to~40-fold increase in the reactivity of nitrate formation reaction driven by ultrasonic energy.A robust semi-continuous N_(2)oxidation by a Ni-mesh-screened cloud system was achieved,providing nitrate with~12 mM concentration every 20 h.These findings emphasize the potential of harnessing the microdroplet-mediated cloud electrochemistry of N_(2)in decentralizing the current mass production of fertilizer.
基金the National Natural Science Foundation of China(22308358,22208346,22421003)IPE Project for Frontier Basic Research(QYJC-2023-05)+1 种基金National Key Research and Development Program(2022YFC3902701)CAS Project for Young Scientists in Basic Research(YSBR-038).
文摘The purity of electronic-grade chemicals significantly impacts electronic components.Although crystallization has been used to purify cerium ammonium nitrate(CAN),the impurity removal mechanism underlying different crystallization parameters remains unclear.Traditional analytical methods of inductively coupled plasma mass spectrometry(ICP-MS)have problems in detecting trace Fe accurately,because of the high concentration of Ce and interference of polyatomic ions.Therefore,this study developed a new method integrating the standard addition and internal standard methods and explored the role of the kinetic energy discrimination mode.This new approach effectively overcomes Ce-related matrix interference and fills the gap in ultra-trace impurity detection.Furthermore,the study investigated the effects of cooling rate,seed mass loading and seed size on the removal of Fe impurity.The seed mass loading affects the average crystal size through regulating secondary nucleation and crystal growth.The removal of Fe in CAN is determined by surface adsorption and agglomeration.Under the condition of the cooling rate of 0.2 K·min^(-1),and addition of 0.5%(mass)600-680 μm seeds,the Fe content is the lowest,at only 0.24 mg·L^(-1),and the Fe removal rate reaches 92.28%.