The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,...The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.展开更多
Nowadays,the majority of the studies on the substitution are focused on cations(such as Y^(3+),Ti^(4+),P^(5+),etc.)in Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)(LATP),while there are few studies on the substitution of anion...Nowadays,the majority of the studies on the substitution are focused on cations(such as Y^(3+),Ti^(4+),P^(5+),etc.)in Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)(LATP),while there are few studies on the substitution of anion O^(2-).In this work,the modified LATP with a series of LiCl(LATPClx,x=0.1,0.2,0.3,0.4)additives is prepared to enhance ionic conductivity.The successful introduction of Cl-makes the length of the c axis decrease from 20.822(2)to 20.792(1)Å,and the bulk conductivity of 2.13×10^(-3) S·cm^(-1) is achieved in LATPCl_(0.3).Moreover,the Al/Ti-O1/Cl1 and Al/Ti-O_(2)/Cl_(2) distance decrease,while the Li1-O_(2)/Cl_(2) distance increases.Lithium ions migrate more easily in the nanochannel of M3-M1-M3.In addition,the LiCl additive increases the relative density and the grain boundary conductivity of LATPClx compounds.Naturally,a higher ionic conductivity of 2.12×10^(–4) S·cm^(-1) and a low activation energy of 0.30 eV are obtained in LATPCl_(0.3).Correspondingly,the symmetric cell exhibits a low overpotential of±50 mV for over 200 h in LATPCl_(0.3).The solid-state Li|LATPCl_(0.3)|NCM811(NCM811=LiNi0.8Co0.1Mn0.1O_(2))battery exhibits high initial capacity 185.1 mAh·g^(-1) with a capacity retention rate of 95.4%after 100 cycles at 0.5 C.This result suggests that LiCl additive is an effective strategy to promote electrochemical properties of LATP solid electrolyte and can be considered for reference to other inorganic solid electrolytes systems.展开更多
Three types of TiO2 nanostructures were synthesized via a facile hydrolysis method at195 °C. Effects of the preparation method and doping with N and F on the crystal structure and photocatalytic performance of Ti...Three types of TiO2 nanostructures were synthesized via a facile hydrolysis method at195 °C. Effects of the preparation method and doping with N and F on the crystal structure and photocatalytic performance of TiO2 were investigated. The nanomaterials were characterized by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller porosimetry, ultraviolet–visible diffuse reflectance spectroscopy and fluorescent emission spectra. Their photo-catalytic activity was examined by the photodegradation of methylene blue in aqueous solution under both ultra-violet and visible light irradiation. The results show that nitrogen and fluorine co-doped anatase TiO2 had the characteristics of a smaller crystalline size, broader light absorption spectrum and lower charge recombination than pure TiO2. Most importantly, more efficient photocatalytic activity under both ultra-violet and visible light was observed. The obtained N–F-TiO2 nanomaterial shows considerable potential for water treatment under sunlight irradiation.展开更多
基金financially supported by the Australian Research Council (Discovery Early Career Researcher Award No. DE190100005)the support of the Australian Research Council (Grant No. FT160100207)the ontinued support from the Queensland University of Technology (QUT) through the centre for Materials Science。
文摘The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.51772239,51972262 and 22005186)the 111 Project(No.B14040).
文摘Nowadays,the majority of the studies on the substitution are focused on cations(such as Y^(3+),Ti^(4+),P^(5+),etc.)in Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)(LATP),while there are few studies on the substitution of anion O^(2-).In this work,the modified LATP with a series of LiCl(LATPClx,x=0.1,0.2,0.3,0.4)additives is prepared to enhance ionic conductivity.The successful introduction of Cl-makes the length of the c axis decrease from 20.822(2)to 20.792(1)Å,and the bulk conductivity of 2.13×10^(-3) S·cm^(-1) is achieved in LATPCl_(0.3).Moreover,the Al/Ti-O1/Cl1 and Al/Ti-O_(2)/Cl_(2) distance decrease,while the Li1-O_(2)/Cl_(2) distance increases.Lithium ions migrate more easily in the nanochannel of M3-M1-M3.In addition,the LiCl additive increases the relative density and the grain boundary conductivity of LATPClx compounds.Naturally,a higher ionic conductivity of 2.12×10^(–4) S·cm^(-1) and a low activation energy of 0.30 eV are obtained in LATPCl_(0.3).Correspondingly,the symmetric cell exhibits a low overpotential of±50 mV for over 200 h in LATPCl_(0.3).The solid-state Li|LATPCl_(0.3)|NCM811(NCM811=LiNi0.8Co0.1Mn0.1O_(2))battery exhibits high initial capacity 185.1 mAh·g^(-1) with a capacity retention rate of 95.4%after 100 cycles at 0.5 C.This result suggests that LiCl additive is an effective strategy to promote electrochemical properties of LATP solid electrolyte and can be considered for reference to other inorganic solid electrolytes systems.
基金financially supported by the Natural Science Foundation of China (No. 51376110)the Natural Science Foundation of Shandong Province (No. ZR2012BQ027)+2 种基金the Program for Youth Science and Technology Star Fund of Jinan (No. 20120123)the Excellent Young Scientist Foundation of Shandong Province (No. BS2011CL005)the Science Development Project of Shandong Provincial (No. 2014GGX104004)
文摘Three types of TiO2 nanostructures were synthesized via a facile hydrolysis method at195 °C. Effects of the preparation method and doping with N and F on the crystal structure and photocatalytic performance of TiO2 were investigated. The nanomaterials were characterized by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller porosimetry, ultraviolet–visible diffuse reflectance spectroscopy and fluorescent emission spectra. Their photo-catalytic activity was examined by the photodegradation of methylene blue in aqueous solution under both ultra-violet and visible light irradiation. The results show that nitrogen and fluorine co-doped anatase TiO2 had the characteristics of a smaller crystalline size, broader light absorption spectrum and lower charge recombination than pure TiO2. Most importantly, more efficient photocatalytic activity under both ultra-violet and visible light was observed. The obtained N–F-TiO2 nanomaterial shows considerable potential for water treatment under sunlight irradiation.
基金supported by the National Natural Science Foundation of China(U2032154)the Key Research and Development Program of Anhui(202004a05020072)+1 种基金Anhui Initiative in Quantum Information Technologies(AHY100000)Anhui Provincial Natural Science Foundation(1908085ME119)。
基金supported by the National Key Research and Development Program of China(2019YFC1907805)the National Natural Science Foundation of China(52004338)+1 种基金Hunan Provincial Natural Science Foundation(2020JJ5696)Guangdong Provincial Department of Natural Resources(2020-011)。
