scispace - formally typeset
Search or ask a question

Showing papers by "Yi Cui published in 2014"


Journal ArticleDOI
TL;DR: The design is inspired by the structure of a pomegranate, where single silicon nanoparticles are encapsulated by a conductive carbon layer that leaves enough room for expansion and contraction following lithiation and delithiation, resulting in superior cyclability and Coulombic efficiency.
Abstract: Silicon is an attractive material for anodes in energy storage devices1,2,3, because it has ten times the theoretical capacity of its state-of-the-art carbonaceous counterpart. Silicon anodes can be used both in traditional lithium-ion batteries and in more recent Li–O2 and Li–S batteries as a replacement for the dendrite-forming lithium metal anodes. The main challenges associated with silicon anodes are structural degradation and instability of the solid-electrolyte interphase caused by the large volume change (∼300%) during cycling, the occurrence of side reactions with the electrolyte, and the low volumetric capacity when the material size is reduced to a nanometre scale4,5,6,7. Here, we propose a hierarchical structured silicon anode that tackles all three of these problems. Our design is inspired by the structure of a pomegranate, where single silicon nanoparticles are encapsulated by a conductive carbon layer that leaves enough room for expansion and contraction following lithiation and delithiation. An ensemble of these hybrid nanoparticles is then encapsulated by a thicker carbon layer in micrometre-size pouches to act as an electrolyte barrier. As a result of this hierarchical arrangement, the solid-electrolyte interphase remains stable and spatially confined, resulting in superior cyclability (97% capacity retention after 1,000 cycles). In addition, the microstructures lower the electrode–electrolyte contact area, resulting in high Coulombic efficiency (99.87%) and volumetric capacity (1,270 mAh cm−3), and the cycling remains stable even when the areal capacity is increased to the level of commercial lithium-ion batteries (3.7 mAh cm−2). A Si anode with hierarchical morphology can accommodate large volume changes, demonstrates high Coulombic efficiency and cyclability as well as an areal capacity comparable to that of commercial Li-ion batteries.

2,094 citations


Journal ArticleDOI
TL;DR: It is shown that coating the lithium metal anode with a monolayer of interconnected amorphous hollow carbon nanospheres helps isolate the lithiumMetal depositions and facilitates the formation of a stable solid electrolyte interphase, indicating that nanoscale interfacial engineering could be a promising strategy to tackle the intrinsic problems of lithiumMetal anode cycling.
Abstract: For future applications in portable electronics, electric vehicles and grid storage, batteries with higher energy storage density than existing lithium ion batteries need to be developed. Recent efforts in this direction have focused on highcapacity electrode materials such as lithium metal, silicon and tin as anodes, and sulphur and oxygen as cathodes. Lithium metal would be the optimal choice as an anode material, because it has the highest specific capacity (3,860 mAh g –1 )a nd the lowest anode potential of all. However, the lithium anode forms dendritic and mossy metal deposits, leading to serious safety concerns and low Coulombic efficiency during charge/discharge cycles. Although advanced characterization techniques have helped shed light on the lithium growth process, effective strategies to improve lithium metal anode cycling remain elusive. Here, we show that coating the lithium metal anode with a monolayer of interconnected amorphous hollow carbon nanospheres helps isolate the lithium metal depositions and facilitates the formation of a stable solid electrolyte interphase. We show that lithium dendrites do not form up to a practical current density of 1 mA cm –2 .T he Coulombic efficiency improves to ∼99% for more than 150 cycles. This is significantly better than the bare unmodified samples, which usually show rapid Coulombic efficiency decay in fewer than 100 cycles. Our results indicate that nanoscale interfacial engineering could be a promising strategy to tackle the intrinsic problems of lithium metal anodes.

1,465 citations


Journal ArticleDOI
TL;DR: A two-step reaction for preparing three-dimensional electrodes composed of CoSe2 nanoparticles grown on carbon fiber paper shows excellent catalytic activity for a hydrogen evolution reaction in an acidic electrolyte, and offers an attractive catalyst material for large-scale water-splitting technology.
Abstract: Development of a non-noble-metal hydrogen-producing catalyst is essential to the development of solar water-splitting devices. Improving both the activity and the stability of the catalyst remains a key challenge. In this Communication, we describe a two-step reaction for preparing three-dimensional electrodes composed of CoSe2 nanoparticles grown on carbon fiber paper. The electrode exhibits excellent catalytic activity for a hydrogen evolution reaction in an acidic electrolyte (100 mA/cm2 at an overpotential of ∼180 mV). Stability tests though long-term potential cycles and extended electrolysis confirm the exceptional durability of the catalyst. This development offers an attractive catalyst material for large-scale water-splitting technology.

1,237 citations


Journal ArticleDOI
TL;DR: This Review discusses some of the recent developments in the design and implementation of such photonic elements in thin-film photovoltaic cells, including nanoscale wires, particles and voids.
Abstract: High-performance photovoltaic cells use semiconductors to convert sunlight into clean electrical power, and transparent dielectrics or conductive oxides as antireflection coatings. A common feature of these materials is their high refractive index. Whereas high-index materials in a planar form tend to produce a strong, undesired reflection of sunlight, high-index nanostructures afford new ways to manipulate light at a subwavelength scale. For example, nanoscale wires, particles and voids support strong optical resonances that can enhance and effectively control light absorption and scattering processes. As such, they provide ideal building blocks for novel, broadband antireflection coatings, light-trapping layers and super-absorbing films. This Review discusses some of the recent developments in the design and implementation of such photonic elements in thin-film photovoltaic cells.

835 citations


Journal ArticleDOI
TL;DR: In this article, the authors used the conducting allotrope of phosphorus, "black phosphorus" as starting materials, and fabricated composites of black phosphorus nanoparticlegraphite by mechanochemical reaction in a high energy mechanical milling process.
Abstract: High specific capacity battery electrode materials have attracted great research attention. Phosphorus as a low-cost abundant material has a high theoretical specific capacity of 2596 mAh/g with most of its capacity at the discharge potential range of 0.4-1.2 V, suitable as anodes. Although numerous research progress have shown other high capacity anodes such as Si, Ge, Sn, and SnO2, there are only a few studies on phosphorus anodes despite its high theoretical capacity. Successful applications of phosphorus anodes have been impeded by rapid capacity fading, mainly caused by large volume change (around 300%) upon lithiation and thus loss of electrical contact. Using the conducting allotrope of phosphorus, "black phosphorus" as starting materials, here we fabricated composites of black phosphorus nanoparticle-graphite by mechanochemical reaction in a high energy mechanical milling process. This process produces phosphorus-carbon bonds, which are stable during lithium insertion/extraction, maintaining excellent electrical connection between phosphorus and carbon. We demonstrated high initial discharge capacity of 2786 mAh·g(-1) at 0.2 C and an excellent cycle life of 100 cycles with 80% capacity retention. High specific discharge capacities are maintained at fast C rates (2270, 1750, 1500, and 1240 mAh·g(-1) at C/5, 1, 2, and 4.5 C, respectively).

728 citations


Journal ArticleDOI
TL;DR: A promising novel electrode design is demonstrated by growing two-dimensional atomic crystal layers including hexagonal boron nitride and graphene directly on Cu metal current collectors to demonstrate stable cycling over 50 cycles with Coulombic efficiency ∼97% in organic carbonate electrolyte.
Abstract: Stable cycling of lithium metal anode is challenging due to the dendritic lithium formation and high chemical reactivity of lithium with electrolyte and nearly all the materials. Here, we demonstrate a promising novel electrode design by growing two-dimensional (2D) atomic crystal layers including hexagonal boron nitride (h-BN) and graphene directly on Cu metal current collectors. Lithium ions were able to penetrate through the point and line defects of the 2D layers during the electrochemical deposition, leading to sandwiched lithium metal between ultrathin 2D layers and Cu. The 2D layers afford an excellent interfacial protection of Li metal due to their remarkable chemical stability as well as mechanical strength and flexibility, resulting from the strong intralayer bonds and ultrathin thickness. Smooth Li metal deposition without dendritic and mossy Li formation was realized. We showed stable cycling over 50 cycles with Coulombic efficiency ∼97% in organic carbonate electrolyte with current density and areal capacity up to the practical value of 2.0 mA/cm(2)and 5.0 mAh/cm(2), respectively, which is a significant improvement over the unprotected electrodes in the same electrolyte.

640 citations


Journal ArticleDOI
TL;DR: This study discovered that conductive Magnéli phase Ti4O7 is highly effective matrix to bind with sulfur species and demonstrates the importance of surface coordination environment for strongly influencing the S-species binding.
Abstract: Lithium–sulfur batteries show fascinating potential for advanced energy storage systems due to their high specific capacity, low-cost, and environmental benignity. However, the shuttle effect and the uncontrollable deposition of lithium sulfide species result in poor cycling performance and low Coulombic efficiency. Despite the recent success in trapping soluble polysulfides via porous matrix and chemical binding, the important mechanism of such controllable deposition of sulfur species has not been well understood. Herein, we discovered that conductive Magneli phase Ti4O7 is highly effective matrix to bind with sulfur species. Compared with the TiO2–S, the Ti4O7–S cathodes exhibit higher reversible capacity and improved cycling performance. It delivers high specific capacities at various C-rates (1342, 1044, and 623 mAh g–1 at 0.02, 0.1, and 0.5 C, respectively) and remarkable capacity retention of 99% (100 cycles at 0.1 C). The superior properties of Ti4O7–S are attributed to the strong adsorption of su...

619 citations


Journal ArticleDOI
TL;DR: In this paper, a conductive polypyrrole (PPy) hydrogel was synthesized via an interfacial polymerization method, and the unique 3D porous nanostructure constructed by interconnected polymer nanospheres endows PPy hydrogels with good mechanical properties and high performance acting as supercapacitor electrodes.
Abstract: Electrochemically active conducting polymers are an important class of materials for applications in energy storage devices such as batteries and supercapacitors, owing to their advantageous features of unique three-dimensional (3D) porous microstructure, high capacitive energy density, scalable synthesis and light weight. Here, we synthesized a nanostructured conductive polypyrrole (PPy) hydrogel via an interfacial polymerization method. The simple synthesis chemistry offers the conductive hydrogel tunable nanostructures and electrochemical performance, as well as scalable processability. Moreover, the unique 3D porous nanostructure constructed by interconnected polymer nanospheres endows PPy hydrogels with good mechanical properties and high performance acting as supercapacitor electrodes with a specific capacitance of ∼380 F g−1, excellent rate capability, and areal capacitance as high as ∼6.4 F cm−2 at a mass loading of 20 mg cm−2.

584 citations


Journal ArticleDOI
14 Apr 2014-ACS Nano
TL;DR: It is proposed that both the high surface area nanostructure and the 2H semiconducting to 1T metallic phase transition of MoS2 are responsible for the outstanding catalytic activity.
Abstract: Molybdenum disulfide (MoS2) with the two-dimensional layered structure has been widely studied as an advanced catalyst for hydrogen evolution reaction (HER). Intercalating guest species into the van der Waals gaps of MoS2 has been demonstrated as an effective approach to tune the electronic structure and consequently improve the HER catalytic activity. In this work, by constructing nanostructured MoS2 particles with largely exposed edge sites on the three-dimensional substrate and subsequently conducting Li electrochemical intercalation and exfoliation processes, an ultrahigh HER performance with 200 mA/cm2 cathodic current density at only 200 mV overpotential is achieved. We propose that both the high surface area nanostructure and the 2H semiconducting to 1T metallic phase transition of MoS2 are responsible for the outstanding catalytic activity. Electrochemical stability test further confirms the long-term operation of the catalyst.

540 citations


Journal ArticleDOI
TL;DR: This work reports, the encapsulation of Li2S cathodes using two-dimensional layered transition metal disulphides that possess a combination of high conductivity and strong binding withLi2S/Li2Sn species and demonstrates a high specific capacity and high areal capacity.
Abstract: Lithium sulphide is a promising battery cathode material, but it suffers from fast capacity decay. Here, the authors demonstrate the use of two-dimensional transition metal disulphides, in contrast to conventional carbon-based materials, for effective encapsulation of the cathode.

529 citations


Journal ArticleDOI
TL;DR: In this article, the role of the separator in the capacity decay of Li-S batteries was investigated and a thin conductive coating was applied to prevent the formation of the inactive S-related species layer.
Abstract: Lithium–sulfur (Li–S) batteries are highly attractive for future generations of portable electronics and electric vehicles due to their high energy density and potentially low cost. In the past decades, various novel electrodes and electrolytes have been tested to improve Li–S battery performance. However, these designs on electrodes and electrolytes have not fully addressed the problem of low cycling stability of Li–S batteries. Here, we show the role of the separator in the capacity decay of the Li–S battery, namely that it can accommodate a large amount of polysulfides inside which then precipitates as a thick layer of inactive S-related species. Using a thin conductive coating on the separator to prevent the formation of the inactive S-related species layer, we show that the specific capacity and cycling stability of the Li–S battery are both improved significantly compared to the battery with a pristine separator. Combining this separator design with a monodisperse sulfur nanoparticle cathode, we show Li–S batteries with a life of over 500 cycles with an initial specific capacity of 1350 mA h g−1 at C/2 and a cycle decay as low as 0.09% per cycle.

Journal ArticleDOI
TL;DR: Sodium manganese hexacyanomanganate, an open-framework crystal structure material, is presented as a viable positive electrode for sodium-ion batteries and provides chemical and structural evidence for the unprecedented storage of 50% more sodium cations than previously thought possible during electrochemical cycling.
Abstract: Potential applications of sodium-ion batteries in grid-scale energy storage, portable electronics and electric vehicles have revitalized research interest in these batteries. However, the performance of sodium-ion electrode materials has not been competitive with that of lithium-ion electrode materials. Here we present sodium manganese hexacyanomanganate (Na2MnII[MnII(CN)6]), an open-framework crystal structure material, as a viable positive electrode for sodium-ion batteries. We demonstrate a high discharge capacity of 209 mAh g−1 at C/5 (40 mA g−1) and excellent capacity retention at high rates in a propylene carbonate electrolyte. We provide chemical and structural evidence for the unprecedented storage of 50% more sodium cations than previously thought possible during electrochemical cycling. These results represent a step forward in the development of sodium-ion batteries. Sodium-ion batteries are considered an alternative to lithium-ion batteries because of easy availability and low cost of sodium. Here, Lee et al.report a manganese hexacyanomanganate material as a sodium-ion battery cathode, which exhibits high discharge capacity.

Journal ArticleDOI
TL;DR: This work demonstrates a safe, fast, inexpensive, long-cycle life aqueous electrolyte battery, which involves the insertion of sodium ions, and reports a newly developed manganese hexacyanomanganate open-framework anode that has the same crystal structure.
Abstract: New types of energy storage are needed in conjunction with the deployment of renewable energy sources and their integration with the electrical grid. We have recently introduced a family of cathodes involving the reversible insertion of cations into materials with the Prussian Blue open-framework crystal structure. Here we report a newly developed manganese hexacyanomanganate open-framework anode that has the same crystal structure. By combining it with the previously reported copper hexacyanoferrate cathode we demonstrate a safe, fast, inexpensive, long-cycle life aqueous electrolyte battery, which involves the insertion of sodium ions. This high rate, high efficiency cell shows a 96.7% round trip energy efficiency when cycled at a 5C rate and an 84.2% energy efficiency at a 50C rate. There is no measurable capacity loss after 1,000 deep-discharge cycles. Bulk quantities of the electrode materials can be produced by a room temperature chemical synthesis from earth-abundant precursors.

Journal ArticleDOI
TL;DR: A method for electrochemical lithium tuning of catalytic materials in organic electrolyte for subsequent enhancement of the catalytic activity in aqueous solution is demonstrated and exhibits a notable performance, better than the benchmark iridium/carbon catalyst.
Abstract: Searching for low-cost and efficient catalysts for the oxygen evolution reaction has been actively pursued owing to its importance in clean energy generation and storage. While developing new catalysts is important, tuning the electronic structure of existing catalysts over a wide electrochemical potential range can also offer a new direction. Here we demonstrate a method for electrochemical lithium tuning of catalytic materials in organic electrolyte for subsequent enhancement of the catalytic activity in aqueous solution. By continuously extracting lithium ions out of LiCoO2, a popular cathode material in lithium ion batteries, to Li0.5CoO2 in organic electrolyte, the catalytic activity is significantly improved. This enhancement is ascribed to the unique electronic structure after the delithiation process. The general efficacy of this methodology is demonstrated in several mixed metal oxides with similar improvements. The electrochemically delithiated LiCo0.33Ni0.33Fe0.33O2 exhibits a notable performance, better than the benchmark iridium/carbon catalyst.

Journal ArticleDOI
TL;DR: In this paper, the authors showed that solid species deposit preferentially onto tin-doped indium oxide instead of carbon during electrochemical charge/discharge of soluble polysuphides.
Abstract: Lithium-sulphur batteries are attractive owing to their high theoretical energy density and reasonable kinetics. Despite the success of trapping soluble polysulphides in a matrix with high surface area, spatial control of solid-state sulphur and lithium sulphide species deposition as a critical aspect has not been demonstrated. Herein, we show a clear visual evidence that these solid species deposit preferentially onto tin-doped indium oxide instead of carbon during electrochemical charge/discharge of soluble polysuphides. To incorporate this concept of spatial control into more practical battery electrodes, we further prepare carbon nanofibers with tin-doped indium oxide nanoparticles decorating the surface as hybrid three-dimensional electrodes to maximize the number of deposition sites. With 12.5 μl of 5 M Li2S8 as the catholyte and a rate of C/5, we can reach the theoretical limit of Li2S8 capacity ~ 1,470 mAh g(-1) (sulphur weight) under the loading of hybrid electrode only at 4.3 mg cm(-2).

PatentDOI
TL;DR: A manufacturing method of a battery electrode includes: (1) mixing Li2S particles with a binder to form a slurry, the binder including at least one of: (a) an ester moiety, (b) an amide mixtures, (c) a ketone mixture, (d) an imine mixture and (e) an ether mixture; and (f) a nitrile mixture as discussed by the authors.
Abstract: A manufacturing method of a battery electrode includes: (1) mixing Li2S particles with a binder to form a slurry, the binder including at least one of: (a) an ester moiety, (b) an amide moiety, (c) a ketone moiety, (d) an imine moiety, (e) an ether moiety, and (f) a nitrile moiety; and (2) disposing the slurry on a current collector.

Journal ArticleDOI
TL;DR: An electrochemical system using a copper hexacyanoferrate cathode and a Cu/Cu(2+) anode to convert heat into electricity, which has low polarization, high charge capacity, moderate temperature coefficients and low specific heat opens a promising way to utilize low-grade heat.
Abstract: Efficient and low-cost thermal energy-harvesting systems are needed to utilize the tremendous low-grade heat sources. Although thermoelectric devices are attractive, its efficiency is limited by the relatively low figure-of-merit and low-temperature differential. An alternative approach is to explore thermodynamic cycles. Thermogalvanic effect, the dependence of electrode potential on temperature, can construct such cycles. In one cycle, an electrochemical cell is charged at a temperature and then discharged at a different temperature with higher cell voltage, thereby converting heat to electricity. Here we report an electrochemical system using a copper hexacyanoferrate cathode and a Cu/Cu(2+) anode to convert heat into electricity. The electrode materials have low polarization, high charge capacity, moderate temperature coefficients and low specific heat. These features lead to a high heat-to-electricity energy conversion efficiency of 5.7% when cycled between 10 and 60 °C, opening a promising way to utilize low-grade heat.

Journal ArticleDOI
TL;DR: A new strategy for improving safety by designing a smart battery that allows internal battery health to be monitored in situ and achieves early detection of lithium dendrites inside batteries through a bifunctional separator, which offers a third sensing terminal in addition to the cathode and anode.
Abstract: Dendrite growth in lithium-based batteries is hazardous as it could cause internal shorts and raise safety concerns. Here, the authors design a bifunctional separator in lithium-ion batteries, which serves as a sensing terminal and is able to detect early dendrite growth inside the batteries.

Journal ArticleDOI
05 May 2014-ACS Nano
TL;DR: A three-dimensional electrode structure based on hydrogen reduced TiO2 with an inverse opal structure that is highly conductive and robust toward electrochemical cycling is reported to achieve both sulfur physical encapsulation and polysulfides binding simultaneously.
Abstract: Sulfur is a cathode material for lithium-ion batteries with a high specific capacity of 1675 mAh/g. The rapid capacity fading, however, presents a significant challenge for the practical application of sulfur cathodes. Two major approaches that have been developed to improve the sulfur cathode performance include (a) fabricating nanostructured conductive matrix to physically encapsulate sulfur and (b) engineering chemical modification to enhance binding with polysulfides and, thus, to reduce their dissolution. Here, we report a three-dimensional (3D) electrode structure to achieve both sulfur physical encapsulation and polysulfides binding simultaneously. The electrode is based on hydrogen reduced TiO2 with an inverse opal structure that is highly conductive and robust toward electrochemical cycling. The relatively enclosed 3D structure provides an ideal architecture for sulfur and polysulfides confinement. The openings at the top surface allow sulfur infusion into the inverse opal structure. In addition,...

Journal ArticleDOI
TL;DR: In this article, the authors demonstrate a spin-coupled valley photocurrent, within an electric double-layer transistor based on WSe2, whose direction and magnitude depend on the degree of circular polarization of the incident radiation and can be further modulated with an external electric field.
Abstract: The valley degree of freedom in layered transition-metal dichalcogenides provides an opportunity to extend the functionalities of spintronics and valleytronics devices. The achievement of spin-coupled valley polarization induced by the non-equilibrium charge-carrier imbalance between two degenerate and inequivalent valleys has been demonstrated theoretically and by optical experiments. However, the generation of a valley and spin current with the valley polarization in transition-metal dichalcogenides remains elusive. Here we demonstrate a spin-coupled valley photocurrent, within an electric-double-layer transistor based on WSe2, whose direction and magnitude depend on the degree of circular polarization of the incident radiation and can be further modulated with an external electric field. This room-temperature generation and electric control of a valley and spin photocurrent provides a new property of electrons in transition-metal dichalcogenide systems, and thereby enables additional degrees of control for quantum-confined spintronic devices. A spin- and valley-polarized photocurrent is generated, in an electric double-layer transistor, with a direction and magnitude that depends on the degree of circular polarization of the incident radiation and on an external electric field.

Journal ArticleDOI
TL;DR: In this article, a three-dimensionalally interconnected hybrid hydrogel system based on carbon nanotube (CNT)-conductive polymer network architecture is reported for high-performance flexible lithium ion battery electrodes.
Abstract: High-performance flexible energy-storage devices have great potential as power sources for wearable electronics. One major limitation to the realization of these applications is the lack of flexible electrodes with excellent mechanical and electrochemical properties. Currently employed batteries and supercapacitors are mainly based on electrodes that are not flexible enough for these purposes. Here, a three-dimensionally interconnected hybrid hydrogel system based on carbon nanotube (CNT)-conductive polymer network architecture is reported for high-performance flexible lithium ion battery electrodes. Unlike previously reported conducting polymers (e.g., polyaniline, polypyrrole, polythiophene), which are mechanically fragile and incompatible with aqueous solution processing, this interpenetrating network of the CNT-conducting polymer hydrogel exibits good mechanical properties, high conductivity, and facile ion transport, leading to facile electrode kinetics and high strain tolerance during electrode volume change. A high-rate capability for TiO2 and high cycling stability for SiNP electrodes are reported. Typically, the flexible TiO2 electrodes achieved a capacity of 76 mAh g–1 in 40 s of charge/discharge and a high areal capacity of 2.2 mAh cm–2 can be obtained for flexible SiNP-based electrodes at 0.1C rate. This simple yet efficient solution process is promising for the fabrication of a variety of high performance flexible electrodes.

Journal ArticleDOI
TL;DR: Li2S is an attractive prelithiated cathode material with a high theoretical capacity of 1166 mA h g−1, which is far above that of its transition metal oxide/phosphate counterparts.
Abstract: Li2S is an attractive prelithiated cathode material with a high theoretical capacity of 1166 mA h g−1, which is far above that of its transition metal oxide/phosphate counterparts. Here, we demonstrate facile, in situ synthesis of Li2S–polypyrrole composites for use as high-performance Li2S cathodes. The N atoms in polypyrrole were found to possess favorable Li–N interaction with Li2S, which enables polypyrrole to bind strongly onto and cover the surface of Li2S to constrain intermediate polysulfides during cycling. Polypyrrole, being a conducting polymer, also helps to facilitate electronic conduction. Using the Li2S–polypyrrole composites as a cathode material, we demonstrate a high discharge capacity of 785 mA h g−1 of Li2S (∼1126 mA h g−1 of S) with stable cycling over prolonged 400 charge/discharge cycles.

Journal ArticleDOI
TL;DR: Two-dimensional layered molybdenum disulfide (MoS2) is used to demonstrate the electrochemical selectivity of edge versus terrace sites for Li-S batteries and hydrogen evolution reaction (HER) and provided clear comparison of HER activity between edge and terraces beyond the previous theoretical prediction and experimental proof.
Abstract: Exploring the chemical reactivity of different atomic sites on crystal surface and controlling their exposures are important for catalysis and renewable energy storage. Here, we use two-dimensional layered molybdenum disulfide (MoS2) to demonstrate the electrochemical selectivity of edge versus terrace sites for Li–S batteries and hydrogen evolution reaction (HER). Lithium sulfide (Li2S) nanoparticles decorates along the edges of the MoS2 nanosheet versus terrace, confirming the strong binding energies between Li2S and the edge sites and guiding the improved electrode design for Li–S batteries. We also provided clear comparison of HER activity between edge and terrace sites of MoS2 beyond the previous theoretical prediction and experimental proof.

Journal ArticleDOI
TL;DR: The LixSi-Li2O core-shell nanoparticles enable the practical implementation of high-performance electrode materials in lithium-ion batteries and are potentially compatible with industrial battery fabrication processes.
Abstract: Rapid progress has been made in realizing battery electrode materials with high capacity and long-term cyclability in the past decade. However, low first-cycle Coulombic efficiency as a result of the formation of a solid electrolyte interphase and Li trapping at the anodes, remains unresolved. Here we report LixSi-Li2O core-shell nanoparticles as an excellent prelithiation reagent with high specific capacity to compensate the first-cycle capacity loss. These nanoparticles are produced via a one-step thermal alloying process. LixSi-Li2O core-shell nanoparticles are processible in a slurry and exhibit high capacity under dry-air conditions with the protection of a Li2O passivation shell, indicating that these nanoparticles are potentially compatible with industrial battery fabrication processes. Both Si and graphite anodes are successfully prelithiated with these nanoparticles to achieve high first-cycle Coulombic efficiencies of 94% to >100%. The LixSi-Li2O core-shell nanoparticles enable the practical implementation of high-performance electrode materials in lithium-ion batteries.

01 May 2014
TL;DR: In this article, an electrochemical system using a copper hexacyanoferrate cathode and a Cu/Cu(2+) anode to convert heat into electricity was presented.
Abstract: Efficient and low-cost thermal energy-harvesting systems are needed to utilize the tremendous low-grade heat sources. Although thermoelectric devices are attractive, its efficiency is limited by the relatively low figure-of-merit and low-temperature differential. An alternative approach is to explore thermodynamic cycles. Thermogalvanic effect, the dependence of electrode potential on temperature, can construct such cycles. In one cycle, an electrochemical cell is charged at a temperature and then discharged at a different temperature with higher cell voltage, thereby converting heat to electricity. Here we report an electrochemical system using a copper hexacyanoferrate cathode and a Cu/Cu(2+) anode to convert heat into electricity. The electrode materials have low polarization, high charge capacity, moderate temperature coefficients and low specific heat. These features lead to a high heat-to-electricity energy conversion efficiency of 5.7% when cycled between 10 and 60 °C, opening a promising way to utilize low-grade heat.

Journal ArticleDOI
TL;DR: A charging-free TREC consisting of an inexpensive soluble Fe(CN)63−/4− redox pair and solid Prussian blue particles as active materials for the two electrodes is demonstrated, which may have potential application for harvesting low-grade heat from the environment, especially in remote areas.
Abstract: Tremendous low-grade heat is stored in industrial processes and the environment. Efficient and low-cost utilization of the low-grade heat is critical to imminent energy and environmental challenges. Here, a rechargeable electrochemical cell (battery) is used to harvest such thermal energy because its voltage changes significantly with temperature. Moreover, by carefully tuning the composition of electrodes, the charging process is purely powered by thermal energy and no electricity is required to charge it. A high heat-to-electricity conversion efficiency of 2.0% can be reached when it is operated between 20 and 60 °C. Such charging-free characteristic may have potential application for harvesting low-grade heat from the environment, especially in remote areas.

Journal ArticleDOI
TL;DR: Electrospinning and electroless deposition is combined to synthesize interconnected, ultralong MNW networks, which opens new opportunities for flexible electronics and roll-to-roll large-scale manufacturing.
Abstract: Metal nanowire (MNW) transparent electrodes have been widely developed for their promising sheet resistance (Rs)–transmittance (T) performance, excellent mechanical flexibility, and facile synthesis. How to lower the junction resistance without compromising optical transmittance has become the key issue in enhancing their performance. Here we combine electrospinning and electroless deposition to synthesize interconnected, ultralong MNW networks. For both silver and copper nanowire networks, the Rs and T values reach around 10 Ω/sq and 90%, respectively. This process is scalable and takes place at ambient temperature and pressure, which opens new opportunities for flexible electronics and roll-to-roll large-scale manufacturing.

Journal ArticleDOI
TL;DR: This study suggests that the electrode performance can be significantly improved by optimizing the electrode geometry, and develops nanoelectrodes made up of nanotubes of iridium oxide that afford much longer intracellular access and are minimally invasive.
Abstract: Intracellular recording of action potentials is important to understand electrically-excitable cells. Recently, vertical nanoelectrodes have been developed to achieve highly sensitive, minimally invasive and large-scale intracellular recording. It has been demonstrated that the vertical geometry is crucial for the enhanced signal detection. Here we develop nanoelectrodes of a new geometry, namely nanotubes of iridium oxide. When cardiomyocytes are cultured upon those nanotubes, the cell membrane not only wraps around the vertical tubes but also protrudes deep into the hollow centre. We show that this nanotube geometry enhances cell-electrode coupling and results in larger signals than solid nanoelectrodes. The nanotube electrodes also afford much longer intracellular access and are minimally invasive, making it possible to achieve stable recording up to an hour in a single session and more than 8 days of consecutive daily recording. This study suggests that the nanoelectrode performance can be significantly improved by optimizing the electrode geometry.

Journal ArticleDOI
TL;DR: A general and scalable synthesis method for porous graphene that is developed through the carbothermal reaction between graphene and metal oxide nanoparticles produced from oxometalates or polyoxometalate is shown.
Abstract: Scalable routes towards porous graphene are useful for developing materials for mass transfer applications. Here, the authors report the fabrication of porous graphene with controllable pore size and nitrogen content via the carbothermal reaction of graphene and (poly)oxometallates.

Journal ArticleDOI
TL;DR: It is shown that light absorption and photocurrent generation in a sub-100 nm active semiconductor layer of a model solar cell can be enhanced by ∼20% over a broad spectral band.
Abstract: The use of a metamaterial mirror in a thin-film solar cell enhances light absorption and photocurrent generation by about 20%.