The hydrogenation of carbon dioxide to produce high-value fuels such as ethanol is currently a research hotspot,but addressing the low selectivity for ethanol remains a challenge.Herein,morphologycontrolled CeO_(2) wi...The hydrogenation of carbon dioxide to produce high-value fuels such as ethanol is currently a research hotspot,but addressing the low selectivity for ethanol remains a challenge.Herein,morphologycontrolled CeO_(2) with different exposed crystal facets,including nanorods(220),nanocubes(200)and nanoplatelets(111),were prepared and impregnated with rhodium(Rh)to obtain Rh/CeO_(2) catalysts,and then the catalytic performance of CO_(2) hydrogenation was investigated.Rh/CeO_(2)-r(nanorods)exhibits high efficacy for CO_(2) hydrogenation to ethanol,giving a high ethanol selectivity of 20.9%with a moderate CO_(2) conversion of 11.2%,and the one-pass ethanol productivity reaches 69.2 mmol/(gRh·h).Characterization results reveal that tuning the exposed crystal facets of the CeO_(2) can tailor the interaction between Rh and CeO_(2),and adjust the chemical state of the Rh species.Due to the abundant oxygen vacancies occupied on the exposed(220)facets of CeO_(2) nanorods,multi-level interactions arise between Rh and CeO_(2)-r,and produce more content of Rh^(+)species.This interface facilitates the transformation of carbonate species into HCOO^(*)and CO^(*)simultaneously,finally boosting the ethanol formation by the C-C coupling reaction.展开更多
The spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO)cathode active materials(CAMs)are considered a promising alternative to commercially available cathodes such as layered and polyanion oxide cathodes,primarily due to their notab...The spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO)cathode active materials(CAMs)are considered a promising alternative to commercially available cathodes such as layered and polyanion oxide cathodes,primarily due to their notable safety and high energy density,particularly in their single-crystal type.Nevertheless,the industrial application of the LNMO CAMs is severely inhibited due to the interfacial deterioration and corrosion under proton-rich and high-voltage conditions.This study successfully designed and synthesized two typical types of crystal facets-exposed single-crystal LNMO CAMs.By tracking the electrochemical deterioration and chemical corrosion evolution,this study elucidates the surface degradation mechanisms and intrinsic instability of the LNMO,contingent upon their crystal facets.The(111)facet,due to its elevated surface energy,is found to be more susceptible to external attack compared to the(100)and(110)facets.Our study highlights the electrochemical corrosion stability of crystal plane engineering for spinel LNMO CAMs.展开更多
A series of Ag2–xO/FTO-i electrodes(where i denotes the current density during the electrodeposition, and i = 0.5, 1, 2, 3, 4, or 7) was fabricated in 0.1 M K2B4O7 electrolyte containing Ag+ ions by galvanostatic ele...A series of Ag2–xO/FTO-i electrodes(where i denotes the current density during the electrodeposition, and i = 0.5, 1, 2, 3, 4, or 7) was fabricated in 0.1 M K2B4O7 electrolyte containing Ag+ ions by galvanostatic electrocrystallization. The electrode composition and morphology were characterized using X-ray powder diffraction, scanning electron microscopy, and X-ray photoelectron spectroscopy. The results reveal that the electrode films consist of Ag2O, but some of the Ag+ ions on the {111} crystal facets are oxidized into Ag2+ ions. Furthermore, the Ag2–xO/FTO-1 electrode shows a triangular slice shape of a parallel matrix with a larger exposed area of {111} crystal facets than other Ag2–xO/FTO-i(i = 0.5, 2, 3, 4, or 7) electrodes. Electrocatalytic experiments prove that the Ag2–xO/FTO-1 electrode produces the highest oxidative current density, has an overpotential of 417 m V at 10 m A cm–2, and has a Tafel slope of 47 m V dec–1 in 0.1 M K2B4O7. Electrochemical impedance spectra indicate that Ag2–xO/FTO-1 electrodes have the best ability for charge transfer. In addition, in the I-t test over 10 h, the current density decreased 4%. Fortunately, both O–O and Ag2+ species were detected after electrocatalysis and a possible mechanism for the oxygen evolution reaction is proposed in which the formation of Ag2+ and O–O species on {111} facets plays a critical role.展开更多
Tuning the exposed crystal facets of{111},{110},and{100}in the spinel LiMn_(2)O_(4)cathode has been proposed to boost their structural stability for advanced lithium-ion batteries.Nevertheless,the role of these varied...Tuning the exposed crystal facets of{111},{110},and{100}in the spinel LiMn_(2)O_(4)cathode has been proposed to boost their structural stability for advanced lithium-ion batteries.Nevertheless,the role of these varied exposed crystal facets on the electrochemical properties is still controversial.Herein,we design octahedral LiMn_(2)O_(4)with only exposed{111}facets and truncated octahedral LiMn_(2)O_(4)(TO-LMO)with exposed{111}and{100}facets.The TO-LMO with different ratios of exposed{100}/{111}facets are prepared by employing the Li-deficient composite as an intermediate phase.展开更多
In direct ethylene glycol fuel cells,advanced anodic electrocatalysts are urgently required to achieve high energy efficiency and optimal fuel utilization for complete ethylene glycol electrooxidation.In this work,bim...In direct ethylene glycol fuel cells,advanced anodic electrocatalysts are urgently required to achieve high energy efficiency and optimal fuel utilization for complete ethylene glycol electrooxidation.In this work,bimetallic PtRh nanodendrites(PtRh NDs)with a three-dimensionally self-supporting structure,abundant(100)crystal facets,and numerous Pt/Rh active sites are synthesized using a simple wet chemical reduction method.The as-synthesized PtRh NDs exhibit outstanding electrocatalytic activity and remarkable selectivity for the ethylene glycol oxidation reaction(EGOR)in alkaline media,significantly enhancing the utilization of ethylene glycol fuel in fuel cells.Theoretical calculations demonstrate that the exposure of(100)crystal faces and the incorporation of Rh atoms play crucial roles in improving the activity and selectivity of EGOR.The present work not only provides an effective method for the synthesis of PtRh NDs with rich(100)crystal faces but also provides new insights into the synergistic effects between the crystal faces and the components in the electrocata lytic process.展开更多
Photocatalytic ozonation holds promise for advanced water purification,yet its development has been hindered by a limited understanding of ozone activation mechanisms and its related photogenerated electron transfer d...Photocatalytic ozonation holds promise for advanced water purification,yet its development has been hindered by a limited understanding of ozone activation mechanisms and its related photogenerated electron transfer dynamics.Herein,we employed in-situ DRIFTS and Raman spectroscopy to elucidate the distinct adsorption and activation behaviors of ozone(O_(3))on the{001}and{110}crystal facets of Bi_(2)O_(2)CO_(3)(BOC)nanosheets.BOC-{001}demonstrates superior photocatalytic ozonation performance,with 85%phenol mineralization and excellent durability,significantly outperforming the 53%mineralization rate of BOC-{110}.This enhanced activity is attributed to non-dissociative ozone adsorption and favorable adsorption energy over{001}facet,which facilitate the one-electron O_(3) reduction pathway.Furthermore,crystal facet engineering strengthens the built-in electric field,promoting exciton dissociation and the generation of localized charge carriers.The synergistic effects of optimized electron availability and ozone adsorption significantly boost the production of reactive oxygen species.These findings provide a deeper understanding of the critical roles of O_(3) adsorption and electron transfer in radical generation,which could provide some guidance for the strategic development of highly effective photocatalytic ozonation catalysts.展开更多
Natural photosynthesis,which provides a green and high-efficiency energy conversion path by spatial separation of photogenerated carriers through combined actions of molecules ingeniously arranged in an efficient sola...Natural photosynthesis,which provides a green and high-efficiency energy conversion path by spatial separation of photogenerated carriers through combined actions of molecules ingeniously arranged in an efficient solar nanospace,highlights the importance of rational nanostructure design to realize artificial high-efficiency photosystem.Inspired by these unique features,we constructed a high-efficiency ternary photosystem by selectively decorating the{001}facets of 18-facet SrTiO_(3)with Au@CdS photosensitizers via a green photo-assisted method.Benefiting from the dual-facilitated charge carriers transportation in core-shell structured Au@CdS heterojunction and well-faceted 18-facet SrTiO_(3)nanocrystal,such a photo-catalyst could realize the effective spatial separation of photogenerated electrons and holes.As expected,the 18-facet SrTiO_(3)/Au@CdS photocatalyst exhibits superior activity in visible-light-driven photocatalytic hydrogen evolution(4.61 mmol h^(−1)g^(−1)),166%improvement in comparison with randomly deposited Au@CdS(1.73 mmol h^(−1)g^(−1)).This work offers new insight into the development of green and high-efficiency photocatalytic systems based on the rational nanostructure design by crystal facet engineering.展开更多
In this work, we report enhanced electroactivity of Co304 nanocrystals （nanocubes, NCs and truncated nano-octahedra, TNO） on the exposed {111} facets as compared to the {001} facets in relation to the surface densit...In this work, we report enhanced electroactivity of Co304 nanocrystals （nanocubes, NCs and truncated nano-octahedra, TNO） on the exposed {111} facets as compared to the {001} facets in relation to the surface density and the activity of the octahedral Com species. Transmission electron microscopy, X-ray powder diffraction, X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy were em- ployed to characterize the crystal facets and materials properties. The enhanced electroactivity of {111 } crystal facets was evaluated by cyclic voltammetry and amperometric titration. Our results indicate that the {111 } facets in TNO has a better electroactivity for enzymeless glucose sensing with a decent glucose sensitivity of 32.54 μA （mmol/L）-1 cm-2.展开更多
Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)has been well demonstrated on electrocatalysts containing single metals but rarely explored...Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems.Here,we synthesize ZnSn(OH)_(6)(ZSO)microcrystals(MCs)with distinct facets and investigate the facet effects in eCO_(2)RR.Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy(in situ-FTIR)reveal that ZSO MCs produce mainly C1 products of HCOOH and CO.The{111}facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency(FE)than that of the{100}facet over a wide range of potentials(-0.9 V∼-1.3 V versus RHE).Density Functional Theory(DFT)calculations elucidate that the{111}facet is favorable to the adsorption/activation of CO_(2)molecules,the formation of intermediate in the rate-determining step,and the desorption of C1 products of CO and HCOOH molecules.展开更多
Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosize...Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosized anatase TiO_(2) exposed(001)facet doubles the capacity compared to the micro-sized sample ascribed to the interfacial Mg^(2+)ion storage.First-principles calculations reveal that the diffusion energy barrier of Mg^(2+)on the(001)facet is significantly lower than those in the bulk phase and on(100)facet,and the adsorption energy of Mg^(2+)on the(001)facet is also considerably lower than that on(100)facet,which guarantees superior interfacial Mg^(2+)storage of(001)facet.Moreover,anatase TiO_(2) exposed(001)facet displays a significantly higher capacity of 312.9 mAh g^(−1) in Mg-Li dual-salt electrolyte compared to 234.3 mAh g^(−1) in Li salt electrolyte.The adsorption energies of Mg^(2+)on(001)facet are much lower than the adsorption energies of Li+on(001)facet,implying that the Mg^(2+)ion interfacial storage is more favorable.These results highlight that controlling the crystal facet of the nanocrystals effectively enhances the interfacial storage of multivalent ions.This work offers valuable guidance for the rational design of high-capacity storage systems.展开更多
Although bismuth vanadate(BiVO4)has been promising as photoanode material for photoelectrochemical water splitting,its charge recombination issue by short charge diffusion length has led to various studies about heter...Although bismuth vanadate(BiVO4)has been promising as photoanode material for photoelectrochemical water splitting,its charge recombination issue by short charge diffusion length has led to various studies about heterostructure photoanodes.As a hole blocking layer of BiVO4,titanium dioxide(TiO_(2)) has been considered unsuitable because of its relatively positive valence band edge and low electrical conductivity.Herein,a crystal facet engineering of TiO_(2) nanostructures is proposed to control band structures for the hole blocking layer of BiVO4 nanodots.We design two types of TiO_(2) nanostructures,which are nanorods(NRs)and nanoflowers(NFs)with different(001)and(110)crystal facets,respectively,and fabricate BiVO4/TiO_(2) heterostructure photoanodes.The BiVO4/TiO_(2) NFs showed 4.8 times higher photocurrent density than the BiVO4/TiO_(2) NRs.Transient decay time analysis and time-resolved photoluminescence reveal the enhancement is attributed to the reduced charge recombination,which is originated from the formation of type II band alignment between BiVO4 nanodots and TiO_(2) NFs.This work provides not only new insights into the interplay between crystal facets and band structures but also important steps for the design of highly efficient photoelectrodes.展开更多
Electrocatalytic CO_(2) conversion has been considered as a promising way to recycle CO_(2) and produce sustainable fuels and chemicals.However,the efficient and highly selective electrochemical reduction of CO_(2) di...Electrocatalytic CO_(2) conversion has been considered as a promising way to recycle CO_(2) and produce sustainable fuels and chemicals.However,the efficient and highly selective electrochemical reduction of CO_(2) directly into multi‐carbon(C_(2+))products remains a great challenge.Herein,we synthesized three type catalysts with different morphologies based on Cu_(2)O nanowires,and studied their morphology and crystal facet reconstruction during the pre‐reduction process.Benefiting from abundant exposure of Cu(100)crystal facet,the nanosheet structure derived Cu catalyst showed a high faradaic efficiency(FE)of 67.5%for C_(2+)products.Additionally,electrocatalytic CO_(2) reduction studies were carried out on Cu(100),Cu(110),and Cu(111)single crystal electrodes,which verified that Cu(100)crystal facets are favorable for the C_(2+)products in electrocatalytic CO_(2) reduction.Our work showed that catalysts would reconstruct during the CO_(2) reduction process and the importance in morphology and crystal facet control to obtain desired products.展开更多
The exploitation of the highly reliable gassensing device for exhaled acetone detection possesses momentous and capacious development prospects in the field of an early noninvasive diabetes diagnosis.Considering that ...The exploitation of the highly reliable gassensing device for exhaled acetone detection possesses momentous and capacious development prospects in the field of an early noninvasive diabetes diagnosis.Considering that the characteristics of crystal facets will impact the gas-sensitive performance,herein three different resistive gas sensors were successfully developed by utilizing the stable α-Fe_(2)O_(3)with different crystal facets as the sensitive materials.The gas-sensitive performance testing results reveal that the(110)crystal faceted α-Fe_(2)O_(3)sensor exhibits relatively superior comprehensive gas sensitivity toward acetone.Particularly,it is worth mentioning that the sensor demonstrates reliable sensitivity,rapid response(25 s)/recovery(3 s)speed,and strong anti-interference capability in detecting 2×10^(-6)acetone for the concentration threshold of diabetes,even when exposed to prolonged periods in variable environments.Furthermore,by simply validating the feasibility of the exhalation diagnosis using the as-prepared gas sensor,the(110)faceted α-Fe_(2)O_(3)gas sensor can effectively discriminate the states of healthy human exhalation and the simulated diabetic exhalation.Through integrating the experimental and theoretical analyses,the superior acetone-sensitive performance of the(110)facetedα-Fe_(2)O_(3)gas sensor can principally be interpreted in correlation with crystal facet-dependent gas adsorption capacity and defect-forming ability.These results not only imply a tremendous application perspective in monitoring acetone gas at sub-ppm concentration,but also open up an effective throughway to develop reliable gas-sensing devices for early non-invasive diabetes screening.展开更多
In-situ obserVation technique has been used to study the growth of fractals,dendrites and faceted crystals in a isothermal thin aqueous soiution film system of Ba(NO),micromorphology of fractals as well as a"phas...In-situ obserVation technique has been used to study the growth of fractals,dendrites and faceted crystals in a isothermal thin aqueous soiution film system of Ba(NO),micromorphology of fractals as well as a"phase diagram"showing the dependence of the pattern formation on the growth conditions have been investigated.展开更多
Nanostructured ceria has attracted much attention in the field of redox catalysts due to the numerous active sites with excellent redox ability.Based on the acidic medium etching strategy,we constructed the strong bin...Nanostructured ceria has attracted much attention in the field of redox catalysts due to the numerous active sites with excellent redox ability.Based on the acidic medium etching strategy,we constructed the strong binding centers(hydroxyl sites and strong acid sites)on the surfaces of nanostructured ceria,which regulate the adsorption process of KA-Oil(the mixture of cyclohexanol and cyclohexanone)and to promote high KA-Oil selectivity in cyclohexane oxidation.The three CeO_(2)(nanocube,nanorod and nanopolyhedron)with different exposed crystal planes were treated by acid etching to change the surface sites and catalytic properties.The transition behavior of surface sites during etching was revealed,abundant strong binding centers were proved to be constructed successfully.And especially for the nanorod treated by acid(Acid@CeO_(2)-NR)with the strongest response for sulfuric acid etching,the strong adsorption of cyclohexanone by strong binding centers was confirmed based on the in-situ DRIFTs.The sulfuric acid etching strategy to enhance the selective oxidation of cyclohexane based on the construction of strong binding centers was proved to be feasible and effective,Acid@CeO_(2)-NR with strongest etching response achieved the dramatic promotion of KA-Oil selectivity from 64.1%to 92.3%.展开更多
Crystal facet engineering is an important strategy for fine-tuning the physical and chemical properties in many fields,which will provide an effective route to fundamentally understand the relationship between the sur...Crystal facet engineering is an important strategy for fine-tuning the physical and chemical properties in many fields,which will provide an effective route to fundamentally understand the relationship between the surface structure and the electron state.Many researchers have worked on the technological performance improvement of noble metal nanoparticles and simple metal oxides by tailoring their crystal facets.Perovskite structure oxides are the most prominent mixed-oxide materials in the field of heterogeneous catalysis due to the acceptable catalytic activity and thermal stability.However,the utilization of perovskite oxides is still limited in comparison with noble metal catalysts because the most stable surface is usually terminated with non-catalytically active crystal facets.High-index facet tailoring may be an effective route to improve the activity of perovskite structure catalysts.So far,only several perovskite oxides have been reported on the crystal facet tailoring with well-defined polyhedral shapes.Herein,we review the recent progress in the facet tailoring arts in perovskite structure oxides.This review begins with a general introduction to facet related physical and chemical behavior and the potential facet-dependent applications.Then,the general principles of crystal growth and facet tailoring will be discussed.The principle for possible grown facets of perovskite structure oxides will be proposed.Various shape growth and facet tailoring of perovskite structure oxides will be reviewed in four parts:(i)tungsten and molybdenum trioxide(A^(0)B+6O_(3));(ii)niobate and tantalite(A^(+1)B^(+5)O_(3));(iii)titanate and zirconate(A^(+2)B^(+4)O_(3));(iv)ferrite,chromite and manganite(A^(+3)B^(+3)O_(3)),including mixed-valence state perovskite compounds.The facet tailoring mechanism in perovskite oxides will be discussed in the next section.Finally,an overview of the promising future of facet dependent applications will be given as a perspective outlook.Fundamental understanding of facet tailoring is expected to open up strategies for the development of highly efficient perovskite oxide materials.展开更多
Two-dimensional layered materials have been universally acknowledged to be promising candidates for alternative precious metals in the field of catalysis.The crystal-facet effect is currently rare in the field of elec...Two-dimensional layered materials have been universally acknowledged to be promising candidates for alternative precious metals in the field of catalysis.The crystal-facet effect is currently rare in the field of electrocatalysis and a deep understanding of the catalytic mechanism of bimetallic highly active crystal facets is critical for fabricating high-performance catalysts,but details are still lacking.Herein,we demonstrated a solvent-induced strategy to manufacture well-defined structured CoNi-layered double hydroxides(LHDs)for highly efficient water electrolysis,and gave a detailed mechanism of catalytic activity towards an enhanced OER.Such considerable improvement in catalytic activity was attributed not only to the synergistic catalytic effect of bimetallic hydroxides,but also to the crystal-facet effect,which is caused by the high density of unsaturated-coordination of surface metal atoms.Consequently,the adsorption energy was enhanced and the activation energy of the target reaction was lowered.These unsaturated coordination surface or edge metal atoms can be easily oxidized to form a great amount of active oxyhydroxides,such as β-NiOOH intermediates.In addition,the adjacent Co sites can also regulate the redox reaction kinetics of Ni(OH)_(2)/NiOOH and synergistically catalyze the OER.展开更多
Single-crystal metals are promising substrates for the epitaxial growth of two-dimensional(2D)materials owing to the absence of grain boundaries and distinctive symmetries.The rich arrangements of atoms on various cry...Single-crystal metals are promising substrates for the epitaxial growth of two-dimensional(2D)materials owing to the absence of grain boundaries and distinctive symmetries.The rich arrangements of atoms on various crystal facets serve as an ideal platform for cutting-edge research on regulating the structures of the as-grown 2D materials.However,it is challenging to obtain large single-crystal metal materials,which hinders the in-depth exploration of single-crystal metal-2D material interface interactions.This review provides a critical summary of the recent progress towards achieving large-area single-crystal metals via anomalous grain growth and epitaxial deposition.Then,crucial roles of single-crystal metal substrates in the controlled growth of 2D materials are highlighted by discussing epitaxial growth of single crystals,rapid and low-temperature preparation,and wrinkle elimination.Finally,a perspective into future research on the preparation of single-crystal metals and 2D materials is provided,which is intended to inspire novel growth frontiers for 2D materials.展开更多
Copper–ceria(Cu O–CeO2) catalysts have been known to be very effective for the oxidation of CO, and their chemical behavior has been extensively studied during the last decades. However, the effect of different CeO2...Copper–ceria(Cu O–CeO2) catalysts have been known to be very effective for the oxidation of CO, and their chemical behavior has been extensively studied during the last decades. However, the effect of different CeO2 crystal surfaces on the catalytic activity of Cu O–CeO2 for the oxidation of CO is still unclear and should be further elucidated. In this study, we deposited 1 wt% Cu on mostly {100}-exposed CeO2 nanocubes(1 Cu Ce NC) and mostly {110}-exposed CeO2 nanorods(1 Cu Ce NR), respectively. Both 1 Cu Ce NC and 1 Cu Ce NR have been used as catalysts for the oxidation of CO and achieved 100% and 50% CO conversion at 130 ℃, respectively. The differences in the catalytic activity of 1 Cu Ce NC and 1 Cu Ce NR were analyzed using temperature-programmed reduction of H2 and temperature-programmed desorption of CO techniques. The results confirmed the excellent reducibility of the 1 Cu Ce NC catalyst, which was attributed to the weak interactions between Cu and the CeO2 support. Moreover, in situ diffuse reflectance infrared Fourier-transform spectroscopy studies indicated that the {100} planes of 1 Cu Ce NC facilitated the generation of active Cu(I) sites, which resulted in the formation of highly reactive Cu(I)-CO species during the oxidation of CO. Both the excellent redox properties and effective CO adsorption capacity of the 1 Cu Ce NC catalyst increased its catalytic reactivity.展开更多
The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery s...The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn_(2)O_(4)that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn_(2)O_(4)(Tr-oh LMO) in which the dominant(111) facets minimize Mn dissolution while a small portion of(100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity(20.25 mg g^(-1)per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn_(2)O_(4)in electrochemical lithium recovery.展开更多
基金Project supported by the Shanghai Local Capacity Building Project(23010504600)。
文摘The hydrogenation of carbon dioxide to produce high-value fuels such as ethanol is currently a research hotspot,but addressing the low selectivity for ethanol remains a challenge.Herein,morphologycontrolled CeO_(2) with different exposed crystal facets,including nanorods(220),nanocubes(200)and nanoplatelets(111),were prepared and impregnated with rhodium(Rh)to obtain Rh/CeO_(2) catalysts,and then the catalytic performance of CO_(2) hydrogenation was investigated.Rh/CeO_(2)-r(nanorods)exhibits high efficacy for CO_(2) hydrogenation to ethanol,giving a high ethanol selectivity of 20.9%with a moderate CO_(2) conversion of 11.2%,and the one-pass ethanol productivity reaches 69.2 mmol/(gRh·h).Characterization results reveal that tuning the exposed crystal facets of the CeO_(2) can tailor the interaction between Rh and CeO_(2),and adjust the chemical state of the Rh species.Due to the abundant oxygen vacancies occupied on the exposed(220)facets of CeO_(2) nanorods,multi-level interactions arise between Rh and CeO_(2)-r,and produce more content of Rh^(+)species.This interface facilitates the transformation of carbonate species into HCOO^(*)and CO^(*)simultaneously,finally boosting the ethanol formation by the C-C coupling reaction.
基金supported by the National Natural Science Foundation of China (52374311)the National Natural Science Foundation of Shaanxi (2022KXJ-146)+3 种基金the Fundamental Research Funds for the Central Universities (D5000230091)Open project of Shaanxi Laboratory of Aerospace Power (2022ZY2-JCYJ-01-09)full-depth-sea battery project (No.2020-XXXX-XX-246-00)the Youth Innovation Team of Shaanxi Universities。
文摘The spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO)cathode active materials(CAMs)are considered a promising alternative to commercially available cathodes such as layered and polyanion oxide cathodes,primarily due to their notable safety and high energy density,particularly in their single-crystal type.Nevertheless,the industrial application of the LNMO CAMs is severely inhibited due to the interfacial deterioration and corrosion under proton-rich and high-voltage conditions.This study successfully designed and synthesized two typical types of crystal facets-exposed single-crystal LNMO CAMs.By tracking the electrochemical deterioration and chemical corrosion evolution,this study elucidates the surface degradation mechanisms and intrinsic instability of the LNMO,contingent upon their crystal facets.The(111)facet,due to its elevated surface energy,is found to be more susceptible to external attack compared to the(100)and(110)facets.Our study highlights the electrochemical corrosion stability of crystal plane engineering for spinel LNMO CAMs.
文摘A series of Ag2–xO/FTO-i electrodes(where i denotes the current density during the electrodeposition, and i = 0.5, 1, 2, 3, 4, or 7) was fabricated in 0.1 M K2B4O7 electrolyte containing Ag+ ions by galvanostatic electrocrystallization. The electrode composition and morphology were characterized using X-ray powder diffraction, scanning electron microscopy, and X-ray photoelectron spectroscopy. The results reveal that the electrode films consist of Ag2O, but some of the Ag+ ions on the {111} crystal facets are oxidized into Ag2+ ions. Furthermore, the Ag2–xO/FTO-1 electrode shows a triangular slice shape of a parallel matrix with a larger exposed area of {111} crystal facets than other Ag2–xO/FTO-i(i = 0.5, 2, 3, 4, or 7) electrodes. Electrocatalytic experiments prove that the Ag2–xO/FTO-1 electrode produces the highest oxidative current density, has an overpotential of 417 m V at 10 m A cm–2, and has a Tafel slope of 47 m V dec–1 in 0.1 M K2B4O7. Electrochemical impedance spectra indicate that Ag2–xO/FTO-1 electrodes have the best ability for charge transfer. In addition, in the I-t test over 10 h, the current density decreased 4%. Fortunately, both O–O and Ag2+ species were detected after electrocatalysis and a possible mechanism for the oxygen evolution reaction is proposed in which the formation of Ag2+ and O–O species on {111} facets plays a critical role.
基金funded by the National Natural Science Foundation of China(52102252)Natural Science Foundation of Shandong Province(ZR2021QB052)Postdoctoral Research Foundation of China(2021T140268).
文摘Tuning the exposed crystal facets of{111},{110},and{100}in the spinel LiMn_(2)O_(4)cathode has been proposed to boost their structural stability for advanced lithium-ion batteries.Nevertheless,the role of these varied exposed crystal facets on the electrochemical properties is still controversial.Herein,we design octahedral LiMn_(2)O_(4)with only exposed{111}facets and truncated octahedral LiMn_(2)O_(4)(TO-LMO)with exposed{111}and{100}facets.The TO-LMO with different ratios of exposed{100}/{111}facets are prepared by employing the Li-deficient composite as an intermediate phase.
基金sponsored by the National Natural Science Foundation of China(22272103)the Programs of Science and Technology of Suzhou in China(ZXL2021448 and SYG202137)+4 种基金Science and Technology Innovation Team of Shaanxi Province(2022TD-35 and 2023-CX-TD-27)the Young Scientist Initiative Project of School of Materials Science and Engineering at Shaanxi Normal University(2024YSIP-MSE-SNNU004)the Fundamental Research Funds for the Central Universities(GK202505036)the Technology Innovation Leading Program of Shaanxi in ChinaSanqin Scholars Innovation Teams in Shaanxi Province in China。
文摘In direct ethylene glycol fuel cells,advanced anodic electrocatalysts are urgently required to achieve high energy efficiency and optimal fuel utilization for complete ethylene glycol electrooxidation.In this work,bimetallic PtRh nanodendrites(PtRh NDs)with a three-dimensionally self-supporting structure,abundant(100)crystal facets,and numerous Pt/Rh active sites are synthesized using a simple wet chemical reduction method.The as-synthesized PtRh NDs exhibit outstanding electrocatalytic activity and remarkable selectivity for the ethylene glycol oxidation reaction(EGOR)in alkaline media,significantly enhancing the utilization of ethylene glycol fuel in fuel cells.Theoretical calculations demonstrate that the exposure of(100)crystal faces and the incorporation of Rh atoms play crucial roles in improving the activity and selectivity of EGOR.The present work not only provides an effective method for the synthesis of PtRh NDs with rich(100)crystal faces but also provides new insights into the synergistic effects between the crystal faces and the components in the electrocata lytic process.
文摘Photocatalytic ozonation holds promise for advanced water purification,yet its development has been hindered by a limited understanding of ozone activation mechanisms and its related photogenerated electron transfer dynamics.Herein,we employed in-situ DRIFTS and Raman spectroscopy to elucidate the distinct adsorption and activation behaviors of ozone(O_(3))on the{001}and{110}crystal facets of Bi_(2)O_(2)CO_(3)(BOC)nanosheets.BOC-{001}demonstrates superior photocatalytic ozonation performance,with 85%phenol mineralization and excellent durability,significantly outperforming the 53%mineralization rate of BOC-{110}.This enhanced activity is attributed to non-dissociative ozone adsorption and favorable adsorption energy over{001}facet,which facilitate the one-electron O_(3) reduction pathway.Furthermore,crystal facet engineering strengthens the built-in electric field,promoting exciton dissociation and the generation of localized charge carriers.The synergistic effects of optimized electron availability and ozone adsorption significantly boost the production of reactive oxygen species.These findings provide a deeper understanding of the critical roles of O_(3) adsorption and electron transfer in radical generation,which could provide some guidance for the strategic development of highly effective photocatalytic ozonation catalysts.
基金This work was financially supported by the Natural Science Foundation of China(Nos.51832003 and 52003212)the Fun-damental Research Funds for the Central University(No.WUT 2020III034).
文摘Natural photosynthesis,which provides a green and high-efficiency energy conversion path by spatial separation of photogenerated carriers through combined actions of molecules ingeniously arranged in an efficient solar nanospace,highlights the importance of rational nanostructure design to realize artificial high-efficiency photosystem.Inspired by these unique features,we constructed a high-efficiency ternary photosystem by selectively decorating the{001}facets of 18-facet SrTiO_(3)with Au@CdS photosensitizers via a green photo-assisted method.Benefiting from the dual-facilitated charge carriers transportation in core-shell structured Au@CdS heterojunction and well-faceted 18-facet SrTiO_(3)nanocrystal,such a photo-catalyst could realize the effective spatial separation of photogenerated electrons and holes.As expected,the 18-facet SrTiO_(3)/Au@CdS photocatalyst exhibits superior activity in visible-light-driven photocatalytic hydrogen evolution(4.61 mmol h^(−1)g^(−1)),166%improvement in comparison with randomly deposited Au@CdS(1.73 mmol h^(−1)g^(−1)).This work offers new insight into the development of green and high-efficiency photocatalytic systems based on the rational nanostructure design by crystal facet engineering.
基金financial support from the University of Queenslandthe support of the Centre for Microscopy and Microanalysis at the University of Queensland through their facilities,and the scientific and technical assistance
文摘In this work, we report enhanced electroactivity of Co304 nanocrystals （nanocubes, NCs and truncated nano-octahedra, TNO） on the exposed {111} facets as compared to the {001} facets in relation to the surface density and the activity of the octahedral Com species. Transmission electron microscopy, X-ray powder diffraction, X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy were em- ployed to characterize the crystal facets and materials properties. The enhanced electroactivity of {111 } crystal facets was evaluated by cyclic voltammetry and amperometric titration. Our results indicate that the {111 } facets in TNO has a better electroactivity for enzymeless glucose sensing with a decent glucose sensitivity of 32.54 μA （mmol/L）-1 cm-2.
基金the Fundamental Research Funds for the Central Universities and the Fundamental Science Research of Harbin Institute of Technology(No.AUGA2160100119,AUGA9803100120,AUGA5710001120).
文摘Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems.Here,we synthesize ZnSn(OH)_(6)(ZSO)microcrystals(MCs)with distinct facets and investigate the facet effects in eCO_(2)RR.Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy(in situ-FTIR)reveal that ZSO MCs produce mainly C1 products of HCOOH and CO.The{111}facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency(FE)than that of the{100}facet over a wide range of potentials(-0.9 V∼-1.3 V versus RHE).Density Functional Theory(DFT)calculations elucidate that the{111}facet is favorable to the adsorption/activation of CO_(2)molecules,the formation of intermediate in the rate-determining step,and the desorption of C1 products of CO and HCOOH molecules.
基金supported by the National Key R&D Program of China(No.2023YFB3809500)the Fundamental Research Funds for the Central Universities(No.2024CDJXY003)+1 种基金the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2023087)The Chongqing Technology Innovation and Application Development Project(No.2024TIAD-KPX0003).
文摘Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosized anatase TiO_(2) exposed(001)facet doubles the capacity compared to the micro-sized sample ascribed to the interfacial Mg^(2+)ion storage.First-principles calculations reveal that the diffusion energy barrier of Mg^(2+)on the(001)facet is significantly lower than those in the bulk phase and on(100)facet,and the adsorption energy of Mg^(2+)on the(001)facet is also considerably lower than that on(100)facet,which guarantees superior interfacial Mg^(2+)storage of(001)facet.Moreover,anatase TiO_(2) exposed(001)facet displays a significantly higher capacity of 312.9 mAh g^(−1) in Mg-Li dual-salt electrolyte compared to 234.3 mAh g^(−1) in Li salt electrolyte.The adsorption energies of Mg^(2+)on(001)facet are much lower than the adsorption energies of Li+on(001)facet,implying that the Mg^(2+)ion interfacial storage is more favorable.These results highlight that controlling the crystal facet of the nanocrystals effectively enhances the interfacial storage of multivalent ions.This work offers valuable guidance for the rational design of high-capacity storage systems.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(2021R1A2B5B03001851)the NRF Grant funded by the Korean government MSIT(2021M3H4A1A03057403).M.G.L.acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education(2021R1A6A3A03039988).J.W.Y.acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education(2021R1A6A3A13046700).
文摘Although bismuth vanadate(BiVO4)has been promising as photoanode material for photoelectrochemical water splitting,its charge recombination issue by short charge diffusion length has led to various studies about heterostructure photoanodes.As a hole blocking layer of BiVO4,titanium dioxide(TiO_(2)) has been considered unsuitable because of its relatively positive valence band edge and low electrical conductivity.Herein,a crystal facet engineering of TiO_(2) nanostructures is proposed to control band structures for the hole blocking layer of BiVO4 nanodots.We design two types of TiO_(2) nanostructures,which are nanorods(NRs)and nanoflowers(NFs)with different(001)and(110)crystal facets,respectively,and fabricate BiVO4/TiO_(2) heterostructure photoanodes.The BiVO4/TiO_(2) NFs showed 4.8 times higher photocurrent density than the BiVO4/TiO_(2) NRs.Transient decay time analysis and time-resolved photoluminescence reveal the enhancement is attributed to the reduced charge recombination,which is originated from the formation of type II band alignment between BiVO4 nanodots and TiO_(2) NFs.This work provides not only new insights into the interplay between crystal facets and band structures but also important steps for the design of highly efficient photoelectrodes.
文摘Electrocatalytic CO_(2) conversion has been considered as a promising way to recycle CO_(2) and produce sustainable fuels and chemicals.However,the efficient and highly selective electrochemical reduction of CO_(2) directly into multi‐carbon(C_(2+))products remains a great challenge.Herein,we synthesized three type catalysts with different morphologies based on Cu_(2)O nanowires,and studied their morphology and crystal facet reconstruction during the pre‐reduction process.Benefiting from abundant exposure of Cu(100)crystal facet,the nanosheet structure derived Cu catalyst showed a high faradaic efficiency(FE)of 67.5%for C_(2+)products.Additionally,electrocatalytic CO_(2) reduction studies were carried out on Cu(100),Cu(110),and Cu(111)single crystal electrodes,which verified that Cu(100)crystal facets are favorable for the C_(2+)products in electrocatalytic CO_(2) reduction.Our work showed that catalysts would reconstruct during the CO_(2) reduction process and the importance in morphology and crystal facet control to obtain desired products.
基金financially supported by the National Natural Science Foundation of China(Nos.62101477,62071410 and 21802114)the Science and Technology Innovation Program of Hunan Province(No.2023RC3133)the Excellent Youth Scholars of Hunan Provincial Department of Education(No.21B0141)。
文摘The exploitation of the highly reliable gassensing device for exhaled acetone detection possesses momentous and capacious development prospects in the field of an early noninvasive diabetes diagnosis.Considering that the characteristics of crystal facets will impact the gas-sensitive performance,herein three different resistive gas sensors were successfully developed by utilizing the stable α-Fe_(2)O_(3)with different crystal facets as the sensitive materials.The gas-sensitive performance testing results reveal that the(110)crystal faceted α-Fe_(2)O_(3)sensor exhibits relatively superior comprehensive gas sensitivity toward acetone.Particularly,it is worth mentioning that the sensor demonstrates reliable sensitivity,rapid response(25 s)/recovery(3 s)speed,and strong anti-interference capability in detecting 2×10^(-6)acetone for the concentration threshold of diabetes,even when exposed to prolonged periods in variable environments.Furthermore,by simply validating the feasibility of the exhalation diagnosis using the as-prepared gas sensor,the(110)faceted α-Fe_(2)O_(3)gas sensor can effectively discriminate the states of healthy human exhalation and the simulated diabetic exhalation.Through integrating the experimental and theoretical analyses,the superior acetone-sensitive performance of the(110)facetedα-Fe_(2)O_(3)gas sensor can principally be interpreted in correlation with crystal facet-dependent gas adsorption capacity and defect-forming ability.These results not only imply a tremendous application perspective in monitoring acetone gas at sub-ppm concentration,but also open up an effective throughway to develop reliable gas-sensing devices for early non-invasive diabetes screening.
文摘In-situ obserVation technique has been used to study the growth of fractals,dendrites and faceted crystals in a isothermal thin aqueous soiution film system of Ba(NO),micromorphology of fractals as well as a"phase diagram"showing the dependence of the pattern formation on the growth conditions have been investigated.
基金supported by National Natural Science Fund for Excellent Young Scholars(22222813)the National Natural Science Foundation of China(22078338)+2 种基金the National Key Research and Development Program of China(2023YFA1506803)the Postdoctoral Fellowship Program of CPSF(GZC20232700)the“Special Research Assistant Project”of the Chinese Academy of Sciences.
文摘Nanostructured ceria has attracted much attention in the field of redox catalysts due to the numerous active sites with excellent redox ability.Based on the acidic medium etching strategy,we constructed the strong binding centers(hydroxyl sites and strong acid sites)on the surfaces of nanostructured ceria,which regulate the adsorption process of KA-Oil(the mixture of cyclohexanol and cyclohexanone)and to promote high KA-Oil selectivity in cyclohexane oxidation.The three CeO_(2)(nanocube,nanorod and nanopolyhedron)with different exposed crystal planes were treated by acid etching to change the surface sites and catalytic properties.The transition behavior of surface sites during etching was revealed,abundant strong binding centers were proved to be constructed successfully.And especially for the nanorod treated by acid(Acid@CeO_(2)-NR)with the strongest response for sulfuric acid etching,the strong adsorption of cyclohexanone by strong binding centers was confirmed based on the in-situ DRIFTs.The sulfuric acid etching strategy to enhance the selective oxidation of cyclohexane based on the construction of strong binding centers was proved to be feasible and effective,Acid@CeO_(2)-NR with strongest etching response achieved the dramatic promotion of KA-Oil selectivity from 64.1%to 92.3%.
基金supported by the National Natural Science Foundation of China(grants 90922034,21131002,and 21201075)the Specialized Research Fund for the Doctoral Program of Higher Education(SRFDP grant 20110061130005).
文摘Crystal facet engineering is an important strategy for fine-tuning the physical and chemical properties in many fields,which will provide an effective route to fundamentally understand the relationship between the surface structure and the electron state.Many researchers have worked on the technological performance improvement of noble metal nanoparticles and simple metal oxides by tailoring their crystal facets.Perovskite structure oxides are the most prominent mixed-oxide materials in the field of heterogeneous catalysis due to the acceptable catalytic activity and thermal stability.However,the utilization of perovskite oxides is still limited in comparison with noble metal catalysts because the most stable surface is usually terminated with non-catalytically active crystal facets.High-index facet tailoring may be an effective route to improve the activity of perovskite structure catalysts.So far,only several perovskite oxides have been reported on the crystal facet tailoring with well-defined polyhedral shapes.Herein,we review the recent progress in the facet tailoring arts in perovskite structure oxides.This review begins with a general introduction to facet related physical and chemical behavior and the potential facet-dependent applications.Then,the general principles of crystal growth and facet tailoring will be discussed.The principle for possible grown facets of perovskite structure oxides will be proposed.Various shape growth and facet tailoring of perovskite structure oxides will be reviewed in four parts:(i)tungsten and molybdenum trioxide(A^(0)B+6O_(3));(ii)niobate and tantalite(A^(+1)B^(+5)O_(3));(iii)titanate and zirconate(A^(+2)B^(+4)O_(3));(iv)ferrite,chromite and manganite(A^(+3)B^(+3)O_(3)),including mixed-valence state perovskite compounds.The facet tailoring mechanism in perovskite oxides will be discussed in the next section.Finally,an overview of the promising future of facet dependent applications will be given as a perspective outlook.Fundamental understanding of facet tailoring is expected to open up strategies for the development of highly efficient perovskite oxide materials.
基金financially supported by the National Natural Science Foundation of China(22162026,22169022)the Shaanxi Provincial Science and Technology Plan Project(2020JQ-792 and 2020JM-546)+3 种基金the Key Laboratory of Education Department of Shaanxi Province(20JS153)the Doctoral Scientific Research Project of Yan’an University(YDBK2018-04)the Scientific Research Project of Yan’an University(YDY2019-24)the Training Program of Innovation and Entrepreneurship for Undergraduates(S202210719129).
文摘Two-dimensional layered materials have been universally acknowledged to be promising candidates for alternative precious metals in the field of catalysis.The crystal-facet effect is currently rare in the field of electrocatalysis and a deep understanding of the catalytic mechanism of bimetallic highly active crystal facets is critical for fabricating high-performance catalysts,but details are still lacking.Herein,we demonstrated a solvent-induced strategy to manufacture well-defined structured CoNi-layered double hydroxides(LHDs)for highly efficient water electrolysis,and gave a detailed mechanism of catalytic activity towards an enhanced OER.Such considerable improvement in catalytic activity was attributed not only to the synergistic catalytic effect of bimetallic hydroxides,but also to the crystal-facet effect,which is caused by the high density of unsaturated-coordination of surface metal atoms.Consequently,the adsorption energy was enhanced and the activation energy of the target reaction was lowered.These unsaturated coordination surface or edge metal atoms can be easily oxidized to form a great amount of active oxyhydroxides,such as β-NiOOH intermediates.In addition,the adjacent Co sites can also regulate the redox reaction kinetics of Ni(OH)_(2)/NiOOH and synergistically catalyze the OER.
基金financially supported by Beijing National Laboratory for Molecular Sciences(BNLMS-CXTD-202001)the Beijing Municipal Science&Technology Commission(No.Z181100004818001 and Z191100000819005)+1 种基金the National Basic Research Program of China(No.2016YFA0200101)the National Natural Science Foundation of China(No.21525310 and 51520105003).
文摘Single-crystal metals are promising substrates for the epitaxial growth of two-dimensional(2D)materials owing to the absence of grain boundaries and distinctive symmetries.The rich arrangements of atoms on various crystal facets serve as an ideal platform for cutting-edge research on regulating the structures of the as-grown 2D materials.However,it is challenging to obtain large single-crystal metal materials,which hinders the in-depth exploration of single-crystal metal-2D material interface interactions.This review provides a critical summary of the recent progress towards achieving large-area single-crystal metals via anomalous grain growth and epitaxial deposition.Then,crucial roles of single-crystal metal substrates in the controlled growth of 2D materials are highlighted by discussing epitaxial growth of single crystals,rapid and low-temperature preparation,and wrinkle elimination.Finally,a perspective into future research on the preparation of single-crystal metals and 2D materials is provided,which is intended to inspire novel growth frontiers for 2D materials.
文摘Copper–ceria(Cu O–CeO2) catalysts have been known to be very effective for the oxidation of CO, and their chemical behavior has been extensively studied during the last decades. However, the effect of different CeO2 crystal surfaces on the catalytic activity of Cu O–CeO2 for the oxidation of CO is still unclear and should be further elucidated. In this study, we deposited 1 wt% Cu on mostly {100}-exposed CeO2 nanocubes(1 Cu Ce NC) and mostly {110}-exposed CeO2 nanorods(1 Cu Ce NR), respectively. Both 1 Cu Ce NC and 1 Cu Ce NR have been used as catalysts for the oxidation of CO and achieved 100% and 50% CO conversion at 130 ℃, respectively. The differences in the catalytic activity of 1 Cu Ce NC and 1 Cu Ce NR were analyzed using temperature-programmed reduction of H2 and temperature-programmed desorption of CO techniques. The results confirmed the excellent reducibility of the 1 Cu Ce NC catalyst, which was attributed to the weak interactions between Cu and the CeO2 support. Moreover, in situ diffuse reflectance infrared Fourier-transform spectroscopy studies indicated that the {100} planes of 1 Cu Ce NC facilitated the generation of active Cu(I) sites, which resulted in the formation of highly reactive Cu(I)-CO species during the oxidation of CO. Both the excellent redox properties and effective CO adsorption capacity of the 1 Cu Ce NC catalyst increased its catalytic reactivity.
基金supported by the National Natural Science Foundation of China (21878133,21908082,22178154)the Natural Science Foundation of Jiangsu Province(BK20190854)+1 种基金the China Postdoctoral Science Foundation(2020M671364,2021M701472)the Science&Technology Foundation of Zhenjiang (GY2020027)。
文摘The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn_(2)O_(4)that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn_(2)O_(4)(Tr-oh LMO) in which the dominant(111) facets minimize Mn dissolution while a small portion of(100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity(20.25 mg g^(-1)per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn_(2)O_(4)in electrochemical lithium recovery.
