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
Developing cost-effective and facile methods to synthesize efficient and stable electrocatalysts for large-scale water splitting is highly desirable but remains a significant challenge.In this study,a facile ambient t...Developing cost-effective and facile methods to synthesize efficient and stable electrocatalysts for large-scale water splitting is highly desirable but remains a significant challenge.In this study,a facile ambient temperature synthesis of hierarchical nickel-iron(oxy)hydroxides nanosheets on iron foam(FF-FN)with both superhydrophilicity and superaerophobicity is reported.Specifically,the as-fabricated FF-FN electrode demonstrates extraordinary oxygen evolution reaction(OER)activity with an ultralow overpotential of 195 mV at 10 mA cm^(-2)and a small Tafel slope of 34 mV dec^(-1)in alkaline media.Further theoretical investigation indicates that the involved lattice oxygen in nickel-iron-based-oxyhydroxide during electrochemical self-reconstruction can significantly reduce the OER reaction overpotential via the dominated lattice oxygen mechanism.The rechargeable Zn-air battery assembled by directly using the as-prepared FF-FN as cathode displays remarkable cycling performance.It is believed that this work affords an economical approach to steer commercial Fe foam into robust electrocatalysts for sustainable energy conversion and storage systems.展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental pollution.Herein,we report a superaero...Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental pollution.Herein,we report a superaerophobic three dimensional(3D)heterostructured nanowrinkles of bimetallic selenides consisting of crystalline NiSe2 and NiFe2Se4 grown on NiFe alloy(NiSe2/NiFe2Se4@NiFe)prepared by a thermal selenization procedure.In this unique 3D heterostructure,numerous nanowrinkles of NiSe2/NiFe2Se4 hybrid with a thickness of ~100 nm are grown on NiFe alloy in a uniform manner.Profiting by the large active surface area and high electronic conductivity,the superaerophobic NiSe2/NiFe2Se4@NiFe heterostructure exhibits excellent electrocatalytic activity and durability towards OER in alkaline media,outputting the low potentials of 1.53 and 1.54 V to achieve ultra-high current densities of 500 and 1000 mA cm^−2,respectively,which is among the most active Ni/Fe-based selenides,and even superior to the benchmark Ir/C catalyst.The in-situ derived FeOOH and NiOOH species from NiSe2/NiFe2Se4@NiFe are deemed to be efficient active sites for OER.展开更多
Multifunctional non-precious catalysts for hydrogen/oxygen evolution reaction(HER/OER) and oxygen reduction reaction(ORR) constitute the bottleneck in the applications in electrochemical overall water splitting(OWS) a...Multifunctional non-precious catalysts for hydrogen/oxygen evolution reaction(HER/OER) and oxygen reduction reaction(ORR) constitute the bottleneck in the applications in electrochemical overall water splitting(OWS) and Zn-air batteries. Herein, a trifunctional electrocatalyst of urchin-like Al,P-codoped Co3O4 microspheres supported on Ni foam(denoted as AP-CONPs/NF) was fabricated via a hydrothermal process and subsequent low-temperature annealing and phosphorization, exhibiting enhanced OER, HER and ORR activities compared with single-doped and undoped samples. Their surface self-organized microstructure and excellent "superaerophobic" feature make a high bubble repellency, which boost diffusion of reactants and electrolyte-electrode intimate contact. The codoping of Al and P elements into Co3O4 betters right the balance among surface chemical state, the increased oxygen vacancies and the promoted charge transfer. Encouraged by these synergistic advantages, the AP-CONPs/NF was further employed as excellent bifunctional electrodes for the OWS(low cell voltage of 1.57 V at 10 mA cm-2) and as air cathode for rechargeable Zn-air batteries(high power density of 89.1 mW cm-2), which demonstrates a great feasibility for practical applications.展开更多
Surface hydrophilicity is considered to have a strong influence on the biological reactions of bone-substituting materials. However, the influence of a hydrophilic surface on osteoconductivity is not completely clear,...Surface hydrophilicity is considered to have a strong influence on the biological reactions of bone-substituting materials. However, the influence of a hydrophilic surface on osteoconductivity is not completely clear, especially for superhydrophilic surfaces. In this study, we conferred superhydrophilic properties on anodized TiO2 coatings using a hydrothermal treatment, and developed a method to maintain this surface until implantation. The osteoconductivity of these coatings was evaluated with in vivo tests. A hydrothermal treatment made the surface of as-anodized samples more hydrophilic, up to a water contact angle of 13 (deg.). Storage in both air and distilled water increased the water contact angle after several days because of the adsorption of hydrocarbon. However, storage in phosphate buffered solution led to a reduction in the water contact angle, because of the adsorption of the inorganic ions in the solution, and the sample retained its high hydrophilicity for a long time. As the water contact angle decreased, the hard tissue formation ratio increased continuously up to 58%, which was about four times higher than the hard tissue formation ratio on as-polished Ti.展开更多
Superhydrophilic–superhydrophobic patterned surfaces constitute a branch of surface chemistry involving the two extreme states of superhydrophilicity and superhydrophobicity combined on the same surface in precise pa...Superhydrophilic–superhydrophobic patterned surfaces constitute a branch of surface chemistry involving the two extreme states of superhydrophilicity and superhydrophobicity combined on the same surface in precise patterns.Such surfaces have many advantages,including controllable wettability,enrichment ability,accessibility,and the ability to manipulate and pattern water droplets,and they offer new functionalities and possibilities for a wide variety of emerging applications,such as microarrays,biomedical assays,microfluidics,and environmental protection.This review presents the basic theory,simplified fabrication,and emerging applications of superhydrophilic–superhydrophobic patterned surfaces.First,the fundamental theories of wettability that explain the spreading of a droplet on a solid surface are described.Then,the fabrication methods for preparing superhydrophilic–superhydrophobic patterned surfaces are introduced,and the emerging applications of such surfaces that are currently being explored are highlighted.Finally,the remaining challenges of constructing such surfaces and future applications that would benefit from their use are discussed.展开更多
Highly hydrophilic materials enable rapid water delivery and salt redissolution in solar-driven seawater desalination. However, the lack of independent floatability inhibits heat localization at the air/water interfac...Highly hydrophilic materials enable rapid water delivery and salt redissolution in solar-driven seawater desalination. However, the lack of independent floatability inhibits heat localization at the air/water interface. In nature, seaweeds with internal gas microvesicles can float near the sea surface to ensure photosynthesis. Here, we have developed a seaweed-inspired, independently floatable, but superhydrophilic (SIFS) solar evaporator. It needs no extra floatation support and can simultaneously achieve continuous water pumping and heat concentration. The evaporator resists salt accumulation, oil pollution, microbial corrosion, and protein adsorption. Densely packed hollow glass microbeads promote intrinsic floatability and heat insulation. Superhydrophilic zwitterionic sulfobetaine hydrogel provides a continuous water supply, redissolves the deposited salt, and endows the SIFS evaporator with excellent anti-fouling properties. With its unprecedented anti-contamination ability, this SIFS evaporator is expected to open a new avenue for designing floatable superhydrophilic materials and solving real-world issues of solar steam generation in complex environmental conditions.展开更多
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
Although tremendous efforts have been paid on electrocatalysts toward efficient electrochemical hydrogen generation,breakthrough is still highly needed in the design and synthesis of wonderful non-precious-metal elect...Although tremendous efforts have been paid on electrocatalysts toward efficient electrochemical hydrogen generation,breakthrough is still highly needed in the design and synthesis of wonderful non-precious-metal electrocatalyst.Herein,a nanovilli Ni2P electrode,which with superaerophobic and superhydropholic can significantly facilitate the mass and electron transfer was constructed via a facial morphology control strategy.Meanwhile,the substitution of sluggish oxygen evolution with urea oxidation,lowering the two-electrode cell voltage to only 1.48 volts to achieve a current density of 10 mA·cm^(-2).Thus,the as-constructed electrode achieves the operation of hydrogen generation by an AA battery.This work sheds new light on the exploration of other high-efficient electrocatalysts for hydrogen generation by using intermittent clean energy.展开更多
Superhydrophilic surfaces have been applied for supercapacitor;however,during energy storage reaction,how the wettability affects the process of electrochemical reaction specifically is still unclear.Herein,we demonst...Superhydrophilic surfaces have been applied for supercapacitor;however,during energy storage reaction,how the wettability affects the process of electrochemical reaction specifically is still unclear.Herein,we demonstrate superhydrophilic surface for promotion of electrochemical reactions by liquid affinity and further explain the mechanism,where the transition of the wettability state caused by the change in surface free energy is the main reason for the obvious increase in specific capacitance.Through citric acid assistance strategy,an intrinsically hydrophobic Ni(OH)_(2)thick nanosheets(HNHTNs,16 nm)can be transitioned into superhydrophilic Ni(OH)_(2)ultrathin nanosheets(SNHUNs,6.8 nm),where the water contact angle was 0°and the surface free energy increased from 8.6to 65.8 mN·m^(-1),implying superhydrophilicity.Compared with HNHTNs,the specific capacitance of SNHUNs is doubled:from 1230 F·g^(-1)(HNHTNs)to 2350 F·g^(-1)(2A·g^(-1))and,even at 20 A·g^(-1),from 833 F·g^(-1)(HNHTNs)to 1670 F·g^(-1).The asymmetric capacitors assembled by SNHUNs and activated carbon show 52.44 Wh·kg^(-1)at 160W·kg^(-1)and excellent stability with~90%retention after5000 cycles(~80%retention after 9500 cycles).The promotion of electrochemical performances is ascribed to the change of surface wettability caused by surface free energy,which greatly increase affinity of electrode to the surrounding liquid environment to reduce the interface resistance and optimize the electron transport path.展开更多
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sponsored by the Guangdong-Hong Kong-Macao Joint Laboratory(grant no.2019B121205001)Macao Science and Technology Development Fund(FDCT)for funding(project no.0098/2020/A2)+2 种基金the support of the National Natural Science Foundation of China(Grant No.52104309)Natural Science Foundation of Hubei Province(2021CFB011)“Macao Young Scholars Program,”China(AM2020004).
文摘Developing cost-effective and facile methods to synthesize efficient and stable electrocatalysts for large-scale water splitting is highly desirable but remains a significant challenge.In this study,a facile ambient temperature synthesis of hierarchical nickel-iron(oxy)hydroxides nanosheets on iron foam(FF-FN)with both superhydrophilicity and superaerophobicity is reported.Specifically,the as-fabricated FF-FN electrode demonstrates extraordinary oxygen evolution reaction(OER)activity with an ultralow overpotential of 195 mV at 10 mA cm^(-2)and a small Tafel slope of 34 mV dec^(-1)in alkaline media.Further theoretical investigation indicates that the involved lattice oxygen in nickel-iron-based-oxyhydroxide during electrochemical self-reconstruction can significantly reduce the OER reaction overpotential via the dominated lattice oxygen mechanism.The rechargeable Zn-air battery assembled by directly using the as-prepared FF-FN as cathode displays remarkable cycling performance.It is believed that this work affords an economical approach to steer commercial Fe foam into robust electrocatalysts for sustainable energy conversion and storage systems.
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金financially supported by the National Natural Science Foundation of China(21922811,51702284,and 21878270)Zhejiang Provincial Natural Science Foundation of China(LR19B060002)the Startup Foundation for Hundred-Talent Program of Zhejiang University.
文摘Cost-effective and stable electrocatalysts with ultra-high current densities for electrochemical oxygen evolution reaction(OER)are critical to the energy crisis and environmental pollution.Herein,we report a superaerophobic three dimensional(3D)heterostructured nanowrinkles of bimetallic selenides consisting of crystalline NiSe2 and NiFe2Se4 grown on NiFe alloy(NiSe2/NiFe2Se4@NiFe)prepared by a thermal selenization procedure.In this unique 3D heterostructure,numerous nanowrinkles of NiSe2/NiFe2Se4 hybrid with a thickness of ~100 nm are grown on NiFe alloy in a uniform manner.Profiting by the large active surface area and high electronic conductivity,the superaerophobic NiSe2/NiFe2Se4@NiFe heterostructure exhibits excellent electrocatalytic activity and durability towards OER in alkaline media,outputting the low potentials of 1.53 and 1.54 V to achieve ultra-high current densities of 500 and 1000 mA cm^−2,respectively,which is among the most active Ni/Fe-based selenides,and even superior to the benchmark Ir/C catalyst.The in-situ derived FeOOH and NiOOH species from NiSe2/NiFe2Se4@NiFe are deemed to be efficient active sites for OER.
基金the National Natural Science Foundation of China(21421001,21573115,21875118)the Natural Science Foundation of Tianjin(17JCYBJC17100,19JCZDJC37700)。
文摘Multifunctional non-precious catalysts for hydrogen/oxygen evolution reaction(HER/OER) and oxygen reduction reaction(ORR) constitute the bottleneck in the applications in electrochemical overall water splitting(OWS) and Zn-air batteries. Herein, a trifunctional electrocatalyst of urchin-like Al,P-codoped Co3O4 microspheres supported on Ni foam(denoted as AP-CONPs/NF) was fabricated via a hydrothermal process and subsequent low-temperature annealing and phosphorization, exhibiting enhanced OER, HER and ORR activities compared with single-doped and undoped samples. Their surface self-organized microstructure and excellent "superaerophobic" feature make a high bubble repellency, which boost diffusion of reactants and electrolyte-electrode intimate contact. The codoping of Al and P elements into Co3O4 betters right the balance among surface chemical state, the increased oxygen vacancies and the promoted charge transfer. Encouraged by these synergistic advantages, the AP-CONPs/NF was further employed as excellent bifunctional electrodes for the OWS(low cell voltage of 1.57 V at 10 mA cm-2) and as air cathode for rechargeable Zn-air batteries(high power density of 89.1 mW cm-2), which demonstrates a great feasibility for practical applications.
文摘Surface hydrophilicity is considered to have a strong influence on the biological reactions of bone-substituting materials. However, the influence of a hydrophilic surface on osteoconductivity is not completely clear, especially for superhydrophilic surfaces. In this study, we conferred superhydrophilic properties on anodized TiO2 coatings using a hydrothermal treatment, and developed a method to maintain this surface until implantation. The osteoconductivity of these coatings was evaluated with in vivo tests. A hydrothermal treatment made the surface of as-anodized samples more hydrophilic, up to a water contact angle of 13 (deg.). Storage in both air and distilled water increased the water contact angle after several days because of the adsorption of hydrocarbon. However, storage in phosphate buffered solution led to a reduction in the water contact angle, because of the adsorption of the inorganic ions in the solution, and the sample retained its high hydrophilicity for a long time. As the water contact angle decreased, the hard tissue formation ratio increased continuously up to 58%, which was about four times higher than the hard tissue formation ratio on as-polished Ti.
基金This work was supported by the Independent Innovation Fund of Tianjin University(Grant No.2022XJS-0003)the National Key Research and Development Program of China(Grant No.2019YFA0905804).
文摘Superhydrophilic–superhydrophobic patterned surfaces constitute a branch of surface chemistry involving the two extreme states of superhydrophilicity and superhydrophobicity combined on the same surface in precise patterns.Such surfaces have many advantages,including controllable wettability,enrichment ability,accessibility,and the ability to manipulate and pattern water droplets,and they offer new functionalities and possibilities for a wide variety of emerging applications,such as microarrays,biomedical assays,microfluidics,and environmental protection.This review presents the basic theory,simplified fabrication,and emerging applications of superhydrophilic–superhydrophobic patterned surfaces.First,the fundamental theories of wettability that explain the spreading of a droplet on a solid surface are described.Then,the fabrication methods for preparing superhydrophilic–superhydrophobic patterned surfaces are introduced,and the emerging applications of such surfaces that are currently being explored are highlighted.Finally,the remaining challenges of constructing such surfaces and future applications that would benefit from their use are discussed.
基金supported by the National Natural Science Foundation of China(21621004,21961132005,22078238,21908160,and 21805204)the Tianjin Natural Science Foundation(19JCQNJC05100 and 20JCQNJC00170)+1 种基金Young Elite Scientists Sponsorship Program by Tianjin(TJSQNTJ-2018-17)the China Postdoctoral Science Foundation(2019M651041).
文摘Highly hydrophilic materials enable rapid water delivery and salt redissolution in solar-driven seawater desalination. However, the lack of independent floatability inhibits heat localization at the air/water interface. In nature, seaweeds with internal gas microvesicles can float near the sea surface to ensure photosynthesis. Here, we have developed a seaweed-inspired, independently floatable, but superhydrophilic (SIFS) solar evaporator. It needs no extra floatation support and can simultaneously achieve continuous water pumping and heat concentration. The evaporator resists salt accumulation, oil pollution, microbial corrosion, and protein adsorption. Densely packed hollow glass microbeads promote intrinsic floatability and heat insulation. Superhydrophilic zwitterionic sulfobetaine hydrogel provides a continuous water supply, redissolves the deposited salt, and endows the SIFS evaporator with excellent anti-fouling properties. With its unprecedented anti-contamination ability, this SIFS evaporator is expected to open a new avenue for designing floatable superhydrophilic materials and solving real-world issues of solar steam generation in complex environmental conditions.
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.
文摘Fluoroalkyl end-capped vinyltrimethoxysilane-<i><span style="font-family:Verdana;">N</span></i><span><span style="font-family:Verdana;">,</span><i><span style="font-family:Verdana;">N</span></i></span><span style="font-family:Verdana;">-dimethylacrylamide cooli</span><span style="font-family:;" "=""><span style="font-family:Verdana;">gomer [R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(CH</span><sub><span style="font-family:Verdana;">2</span></sub><span style="font-family:Verdana;">-CHSi(OMe)</span><sub><span style="font-family:Verdana;">3</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">x</span></sub></i><span style="font-family:Verdana;">-(CH</span><sub><span style="font-family:Verdana;">2</span></sub><span style="font-family:Verdana;">-CHC(=O)NMe</span><sub><span style="font-family:Verdana;">2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">y</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">;R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;"> = CF(CF</span><sub><span style="font-family:Verdana;">3</span></sub><span style="font-family:Verdana;">)OC</span><sub><span style="font-family:Verdana;">3</span></sub><span style="font-family:Verdana;">F</span><sub><span style="font-family:Verdana;">7</span></sub><span style="font-family:Verdana;">:</span></span><span style="font-family:;" "=""><span style="font-family:Verdana;"> R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM)</span><i><sub><span style="font-family:Verdana;">x</span></sub></i><span style="font-family:Verdana;">-(DMAA)</span><i><sub><span style="font-family:Verdana;">y</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">] was synthesized by reaction of fluoroalkanoyl peroxide [R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-C(=O)O-O(O=)C-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">] with vinyltrimethoxysilane (VM) and </span><i><span style="font-family:Verdana;">N</span></i><span><span style="font-family:Verdana;">,</span><i><span style="font-family:Verdana;">N</span></i></span><span style="font-family:Verdana;">-</span></span><span style="font-family:Verdana;">dimethylacrylamide (DMAA). The modified glass surface treated with the</span><span style="font-family:;" "=""><span style="font-family:Verdana;"> cooligomeric nanoparticles [R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM-SiO</span><sub><span style="font-family:Verdana;">3/2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">x</span></sub></i><span style="font-family:Verdana;">-(DMAA)</span><i><sub><span style="font-family:Verdana;">y</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">] prepared under the sol-gel reaction of the cooligomer under alkaline conditions was found to exhibit an oleophobic/superhydrophilic property, although the corresponding fluorinated homooligomeric nanoparticles [R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM-SiO</span><sub><span style="font-family:Verdana;">3/2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">n</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">] afforded an </span><span style="font-family:Verdana;">oleophobic/hydrophobic property on the modified surface under similar </span><span style="font-family:Verdana;">con</span><span><span style="font-family:Verdana;">ditions. R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM-SiO</span><sub><span style="font-family:Verdana;">3/2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">n</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">/R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM-SiO</span><sub><span style="font-family:Verdana;">3/2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">x</span></sub></i><span style="font-family:Verdana;">-(DMAA)</span><i><sub><span style="font-family:Verdana;">y</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">/</span><b><i><span style="font-family:Verdana;">PSt</span></i></b><span style="font-family:Verdana;"> (micro-sized</span></span> <span style="font-family:Verdana;">polystyrene particles) composites, which were prepared by the sol-gel reac</span><span style="font-family:Verdana;">tions of the corresponding homooligomer and cooligomer in the presence of </span><b><i><span style="font-family:Verdana;">PSt </span></i></b><span style="font-family:Verdana;">particle under alkaline conditions, provided an oleophobic/superhydrophilic </span><span style="font-family:Verdana;">property on the modified surface. However, it was demonstrated that the</span><span><span style="font-family:Verdana;"> surface wettability on the modified surface treated with the R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM-</span></span><span><span style="font-family:Verdana;">SiO</span><sub><span style="font-family:Verdana;">3/2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">n</span></sub></i><span style="font-family:Verdana;">-</span></span></span><span style="font-family:;" "=""><span style="font-family:Verdana;">R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">/R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM-SiO</span><sub><span style="font-family:Verdana;">3/2</span></sub><span style="font-family:Verdana;">)</span><i><sub><span style="font-family:Verdana;">x</span></sub></i><span style="font-family:Verdana;">-(DMAA)</span><i><sub><span style="font-family:Verdana;">y</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">/</span><b><i><span style="font-family:Verdana;">PSt</span></i></b><span style="font-family:Verdana;"> composites changes dramatically from oleophobic/superhydrophilic to superoleophilic/superhydrophilic </span><span style="font-family:Verdana;">and superoleophilic/superhydrophobic characteristics, increasing with </span><span style="font-family:Verdana;">greater </span><span><span style="font-family:Verdana;">feed ratios (mg/mg) of the R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;">-(VM)</span><i><sub><span style="font-family:Verdana;">n</span></sub></i><span style="font-family:Verdana;">-R</span><sub><span style="font-family:Verdana;">F</span></sub><span style="font-family:Verdana;"> homooligomer in homooligo</span></span><span style="font-family:Verdana;">mer/cooligo</span></span><span style="font-family:Verdana;">mer from 0 to 100 in the preparation of the composites. Such controlled surfac</span>
基金the National Natural Science Foundation of China(Nos.21761004,21701035)the Natural Science Foundation of Guangxi(Nos.2018GXNSFBA281085,2018GXNSFAA138126)+3 种基金Specific research project of Guangxi for research bases and talents(Nos.AD18126002,AD18126005)the foundation ability enhancement project of young teachers in Guangxi universities(No.2018KY0163)the Guangxi University for Nationalities Graduate Education Innovation Project(No.gxun-chxzs201916)the 100 Talents Program for Introducing Overseas High-level Talents into Universities of Guangxi and the training program for thousands of backbone young teachers in Guangxi universities.
文摘Although tremendous efforts have been paid on electrocatalysts toward efficient electrochemical hydrogen generation,breakthrough is still highly needed in the design and synthesis of wonderful non-precious-metal electrocatalyst.Herein,a nanovilli Ni2P electrode,which with superaerophobic and superhydropholic can significantly facilitate the mass and electron transfer was constructed via a facial morphology control strategy.Meanwhile,the substitution of sluggish oxygen evolution with urea oxidation,lowering the two-electrode cell voltage to only 1.48 volts to achieve a current density of 10 mA·cm^(-2).Thus,the as-constructed electrode achieves the operation of hydrogen generation by an AA battery.This work sheds new light on the exploration of other high-efficient electrocatalysts for hydrogen generation by using intermittent clean energy.
基金financially supported by the National Natural Science Foundation of China(Nos.22278349 and 62071413)Hebei Natural Science Foundation(Nos.B2020203013 and F2020203056)+4 种基金the Science and Technology Project of Hebei Education Department(No.QN2020137)Subsidy for Hebei Key Laboratory of Applied Chemistry after Operation Performance(No.22567616H)the Cultivation Project for Basic Research Innovation of Yanshan University(No.2021LGZD015)the Natural Science Foundation of Heilongjiang Province of China(No.LH2022B025)the Fundamental Research Funds for the Provincial Universities of Heilongjiang Province(No.KYYWF10236190104)。
文摘Superhydrophilic surfaces have been applied for supercapacitor;however,during energy storage reaction,how the wettability affects the process of electrochemical reaction specifically is still unclear.Herein,we demonstrate superhydrophilic surface for promotion of electrochemical reactions by liquid affinity and further explain the mechanism,where the transition of the wettability state caused by the change in surface free energy is the main reason for the obvious increase in specific capacitance.Through citric acid assistance strategy,an intrinsically hydrophobic Ni(OH)_(2)thick nanosheets(HNHTNs,16 nm)can be transitioned into superhydrophilic Ni(OH)_(2)ultrathin nanosheets(SNHUNs,6.8 nm),where the water contact angle was 0°and the surface free energy increased from 8.6to 65.8 mN·m^(-1),implying superhydrophilicity.Compared with HNHTNs,the specific capacitance of SNHUNs is doubled:from 1230 F·g^(-1)(HNHTNs)to 2350 F·g^(-1)(2A·g^(-1))and,even at 20 A·g^(-1),from 833 F·g^(-1)(HNHTNs)to 1670 F·g^(-1).The asymmetric capacitors assembled by SNHUNs and activated carbon show 52.44 Wh·kg^(-1)at 160W·kg^(-1)and excellent stability with~90%retention after5000 cycles(~80%retention after 9500 cycles).The promotion of electrochemical performances is ascribed to the change of surface wettability caused by surface free energy,which greatly increase affinity of electrode to the surrounding liquid environment to reduce the interface resistance and optimize the electron transport path.