Superhydrophilic surfaces were fabricated on copper substrates by an electrochemical deposition and sintering process. Superhydrophobic surfaces were prepared by constructing micro/nano-structure on copper substrates ...Superhydrophilic surfaces were fabricated on copper substrates by an electrochemical deposition and sintering process. Superhydrophobic surfaces were prepared by constructing micro/nano-structure on copper substrates through an electrochemical deposition method. Conversion from superhydrophobic to superhydrophilic was obtained via a suitable sintering process. After reduction sintering, the contact angle of the superhydrophilic surfaces changed from 155° to 0°. The scanning electron microscope (SEM) images show that the morphology of superhydrophobic and superhydrophilic surfaces looks like corals and cells respectively. The chemical composition and crystal structure of these surfaces were examined using energy dispersive spectrometry (EDS) and X-ray diffraction (XRD). The results show that the main components on superhydrophobic surfaces are Cu, Cu2O and CuO, while the superhydrophilic surfaces are composed of Cu merely. The crystal structure is more inerratic and the grain size becomes bigger after the sintering. The interracial strength of the superhydrophilic surfaces was investigated, showing that the interfacial strength between superhydrophilic layer and copper substrate is considerably high.展开更多
Conferring surfaces with superhydrophilic/superaerophobic characteristics is desirable for synthesizing efficient gas reaction catalysts.However,complicated procedures,high costs,and poor interfaces hinder commerciali...Conferring surfaces with superhydrophilic/superaerophobic characteristics is desirable for synthesizing efficient gas reaction catalysts.However,complicated procedures,high costs,and poor interfaces hinder commercialization.Here,an integrated electrode with tunable wettability derived from a hierarchically porous wood scaffold was well designed for urea oxidation reaction(UOR).Interestingly,the outer surface of the wood lumen was optimized to the preferred wettability via stoichiometry to promote electrolyte permeation and gas escape.This catalyst exhibits outstanding activity and durability for UOR in alkaline media,requiring only a potential of 1.36 V(vs.RHE)to deliver 10 m A cm^(-2)and maintain its activity without significant decay for 60 h.These experiments and theoretical calculations demonstrate that the nickel(oxy)hydroxide layer formed through surface reconstruction of nickel nanoparticles improves the active sites and intrinsic activity.Moreover,the superwetting properties of the electrode promote mass transfer by guaranteeing substantial contact with the electrolyte and accelerating the separation of gaseous products during electrocatalysis.These findings provide the understanding needed to manipulate the surface wettability through rational design and fabrication of efficient electrocatalysts for gas-evolving processes.展开更多
Bubbles are known to affect energy and mass transfer in gas-evolving electrodes,including those in water splitting,chlorine generation,direct methanol fuel cells,and carbon dioxide generation.As bubbles vigorously evo...Bubbles are known to affect energy and mass transfer in gas-evolving electrodes,including those in water splitting,chlorine generation,direct methanol fuel cells,and carbon dioxide generation.As bubbles vigorously evolve in electrochemical reactions,undesired blockage of active sites and ion conducting pathways result in serious energy losses.Since new advances are made with the development of new theories,materials,and techniques,this review discusses the recent works on promoting bubble removal in electrochemical systems with the aim of guiding and motivating future research in this area.We first provide the mechanism of bubble evolution in electrochemical systems and the resultant overpotentials in detail.Then,recent advances in mitigating bubble issues are presented from the perspectives of passive and active strategies.Passive strategies act on the macro-and micro-structures of the electrode,surface wettability,and electrolyte properties.Active strategies employ out-fields,including flowing electrolytes,acoustic fields,magnetic forces,and photothermal effects,to guide bubbles out of reaction sites aiming at high reaction rates,whereas external energy is needed.Finally,the pros and cons of both strategies and future outlooks are presented.This review leads to design guidelines for highperformance gas-evolving electrochemical systems.展开更多
对高效催化剂进行多尺度调控可优化中间体的吸附能量(原子层面),并实现快速传质(三维宏观层面),这对于提升整体水分解性能至关重要.在本工作中,我们首先在镍铁氢氧化物中引入氧空位,然后通过磷化反应将其转化为具有纳米阵列形态的NiFe-V...对高效催化剂进行多尺度调控可优化中间体的吸附能量(原子层面),并实现快速传质(三维宏观层面),这对于提升整体水分解性能至关重要.在本工作中,我们首先在镍铁氢氧化物中引入氧空位,然后通过磷化反应将其转化为具有纳米阵列形态的NiFe-Vo-P催化剂.在析氧反应催化过程中,NiFe-Vo-P表面会原位形成磷酸盐阴离子及具有催化活性的Ni(Fe)OOH,能显著优化反应中间体的吸附强度.结果表明,NiFeVo-P在过电位为289 mV时电流密度可达1.5 A cm^(-2).同时,其超亲水/超疏气纳米阵列形貌可有效促进传质,在25和70℃的条件下,可在~2.0V的电池电压下分别获得580 mA cm^(-2)和1.0 A cm^(-2)的电流密度,是未进行超疏气形貌工程催化剂的电流密度的2倍以上.展开更多
基金Supported by the National Natural Science Foundation of China(51275180)the Fundamental Research Funds for the Central Universities(2013ZM0003)the Doctorate Dissertation Funds of Guangdong Province(sybzzxm 201213)
文摘Superhydrophilic surfaces were fabricated on copper substrates by an electrochemical deposition and sintering process. Superhydrophobic surfaces were prepared by constructing micro/nano-structure on copper substrates through an electrochemical deposition method. Conversion from superhydrophobic to superhydrophilic was obtained via a suitable sintering process. After reduction sintering, the contact angle of the superhydrophilic surfaces changed from 155° to 0°. The scanning electron microscope (SEM) images show that the morphology of superhydrophobic and superhydrophilic surfaces looks like corals and cells respectively. The chemical composition and crystal structure of these surfaces were examined using energy dispersive spectrometry (EDS) and X-ray diffraction (XRD). The results show that the main components on superhydrophobic surfaces are Cu, Cu2O and CuO, while the superhydrophilic surfaces are composed of Cu merely. The crystal structure is more inerratic and the grain size becomes bigger after the sintering. The interracial strength of the superhydrophilic surfaces was investigated, showing that the interfacial strength between superhydrophilic layer and copper substrate is considerably high.
基金financially supported by the National Natural Science Foundation of China(31922057)the Young Elite Scientists Sponsorship Program from National Forestry and Grassland Administration of China(2019132614)+2 种基金the Outstanding Innovative Youth Training Program of Changsha(KQ2106050)The Hunan Provincial Innovation Foundation for Postgraduate(CX20210847)the Scientific Innovation Fund for Graduate of Central South University of Forestry and Technology(CX202101019)。
文摘Conferring surfaces with superhydrophilic/superaerophobic characteristics is desirable for synthesizing efficient gas reaction catalysts.However,complicated procedures,high costs,and poor interfaces hinder commercialization.Here,an integrated electrode with tunable wettability derived from a hierarchically porous wood scaffold was well designed for urea oxidation reaction(UOR).Interestingly,the outer surface of the wood lumen was optimized to the preferred wettability via stoichiometry to promote electrolyte permeation and gas escape.This catalyst exhibits outstanding activity and durability for UOR in alkaline media,requiring only a potential of 1.36 V(vs.RHE)to deliver 10 m A cm^(-2)and maintain its activity without significant decay for 60 h.These experiments and theoretical calculations demonstrate that the nickel(oxy)hydroxide layer formed through surface reconstruction of nickel nanoparticles improves the active sites and intrinsic activity.Moreover,the superwetting properties of the electrode promote mass transfer by guaranteeing substantial contact with the electrolyte and accelerating the separation of gaseous products during electrocatalysis.These findings provide the understanding needed to manipulate the surface wettability through rational design and fabrication of efficient electrocatalysts for gas-evolving processes.
基金P.Tan thanks the funding support from Anhui Provincial Natural Science Foundation(2008085ME155)National Innovative Talents Program(GG2090007001)+1 种基金Chinese Academy of Sciences(CAS)Program(KJ2090130001)USTC Startup Program(KY2090000044).
文摘Bubbles are known to affect energy and mass transfer in gas-evolving electrodes,including those in water splitting,chlorine generation,direct methanol fuel cells,and carbon dioxide generation.As bubbles vigorously evolve in electrochemical reactions,undesired blockage of active sites and ion conducting pathways result in serious energy losses.Since new advances are made with the development of new theories,materials,and techniques,this review discusses the recent works on promoting bubble removal in electrochemical systems with the aim of guiding and motivating future research in this area.We first provide the mechanism of bubble evolution in electrochemical systems and the resultant overpotentials in detail.Then,recent advances in mitigating bubble issues are presented from the perspectives of passive and active strategies.Passive strategies act on the macro-and micro-structures of the electrode,surface wettability,and electrolyte properties.Active strategies employ out-fields,including flowing electrolytes,acoustic fields,magnetic forces,and photothermal effects,to guide bubbles out of reaction sites aiming at high reaction rates,whereas external energy is needed.Finally,the pros and cons of both strategies and future outlooks are presented.This review leads to design guidelines for highperformance gas-evolving electrochemical systems.
基金supported by the National Key R&D Program of China(2021YFB3801301)the National Natural Science Foundation of China(22075076 and 22005098)the Central Government Funds for Guiding Local Science and Technology Development(2021Szvup040)。
文摘对高效催化剂进行多尺度调控可优化中间体的吸附能量(原子层面),并实现快速传质(三维宏观层面),这对于提升整体水分解性能至关重要.在本工作中,我们首先在镍铁氢氧化物中引入氧空位,然后通过磷化反应将其转化为具有纳米阵列形态的NiFe-Vo-P催化剂.在析氧反应催化过程中,NiFe-Vo-P表面会原位形成磷酸盐阴离子及具有催化活性的Ni(Fe)OOH,能显著优化反应中间体的吸附强度.结果表明,NiFeVo-P在过电位为289 mV时电流密度可达1.5 A cm^(-2).同时,其超亲水/超疏气纳米阵列形貌可有效促进传质,在25和70℃的条件下,可在~2.0V的电池电压下分别获得580 mA cm^(-2)和1.0 A cm^(-2)的电流密度,是未进行超疏气形貌工程催化剂的电流密度的2倍以上.