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Li, Matthew

Publications and source records attributed to Li, Matthew.

At least 55 records · Page 3

Strain-Modulated Platinum–Palladium Nanowires for Oxygen Reduction Reaction

Electrocatalytic activity of alloy nanocatalytsts can be manipulated effectively by tuning their physical properties (ensemble, geometric, and ligand effects) to afford optimal surface structure and compositions for proton exchange membrane fuel cell (PEMFC) application. Herein, highly catalytic platinum-palladium nanowires (Pt n Pd 100-n NWs) with a subtle lattice strain and Boerdijk-Coxeter helix type morphology are synthesized through a surfactant-free, thermal single phase solvent method. X-ray diffraction results show that Pt n Pd 100-n NWs are exposed through the (111) facets and their shrinking or expanding lattice parameters can be modulated by the alloy compositions. Electrochemical results reveal that their high catalytic activity correlates with the lattice shrinking, facets, and bimetallic compositions, showing higher activity when the ratio of Pt and Pd is similar to ~78:22, which is further supported by DFT results. Compared to the nanoparticle type platinum-palladium alloyed catalysts with similar metal compositions (Pt n Pd 100-n NPs), the Pt n Pd 100-n NWs exhibit significantly improved electrocatalytic activity and stability for the oxygen reduction reaction. Our findings open new strategies to design the highly active and stable alloy nanocatalysts with controllable compositions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Design strategies for nonaqueous multivalent-ion and monovalent-ion battery anodes

The inability of current battery technologies to keep up with the performance requirements of industry is pushing forward developments in electrochemistry. Specifically, the battery's negative electrode, the anode, presents many unique chemical, physical and engineering challenges. Lithium-based battery technologies have dominated the past decade, but concerns about the limited supply of lithium in the Earth's crust have led researchers to look towards alternative metal-ion technologies. Furthermore, various alkali metals (such as sodium and potassium) and alkali earth metals (such as magnesium and calcium) have attracted significant research interest. In this Review, we analyse these technologies in a coherent manner, addressing the problems of each type of anode, rather than those of specific types of metal-ion batteries. Covering direct metal plating and stripping, intercalation-based, alloy-based and conversion-reaction-based anode technologies, this analysis will offer the reader a comprehensive understanding of the behaviour of different metal-ion anodes and of what can be learned by transferring knowledge between these different systems. Increasing demand for energy-storage systems will inevitably stress the Earth's lithium supply; thus, the research focus is shifting towards other alkali and alkali earth metals. In summary, this Review compares and connects strategies to enable different multivalent and monovalent metal-ion battery anodes, including metal anodes and intercalation-based, alloy-based and conversion-reaction-based anodes.

36 MATERIALS SCIENCE↗

New Concepts in Electrolytes

Over the past decades, Li-ion battery (LIB) has turned into one of the most important advances in the history of technology due to its extensive and in-depth impact on our life. Its omnipresence in all electric vehicles, consumer electronics and electric grids relies on the precisely tuned electrochemical dynamics and interactions among the electrolytes and the diversified anode and cathode chemistries therein. Furthermore, with consumers' demand for battery performance ever increasing, more and more stringent requirements are being imposed upon the established equilibria among these LIB components, and it became clear that the state-of-the-art electrolyte systems could no longer sustain the desired technological trajectory. Driven by such gap, researchers started to explore more unconventional electrolyte systems. From superconcentrated solvent-in-salt electrolytes to solid-state electrolytes, the current research realm of novel electrolyte systems has grown to unprecedented levels. In this review, we will avoid discussions on current state-of-the-art electrolytes but instead focus exclusively on unconventional electrolyte systems that represent new concepts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Crystal-growth-dominated fabrication of metal-organic frameworks with orderly distributed hierarchical porosity

Constructing architectures with hierarchical porosity has been widely considered as the most efficient way to bypass the problems related to slow mass transfer and inaccessibility of internal space in MOFs. Now, a crystal-growth-dominated strategy is proposed to fabricate hierarchically porous MOFs (HP-MOFs). When the crystal growth is dominated by the monomer attachment, the aggregation of nonionic surfactant or polymer can be easily captured and released during the crystal growth process, resulting in the formation and ordering hierarchical pores along the radial direction. Furthermore, owing to the accelerated mass diffusion and more exposed active sites of this design, HP-MOFs exhibited an enhanced catalytic efficiency in styrene oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Selective Growth of a Discontinuous Subnanometer Pd Film on Carbon Defects for Li–O 2 Batteries

A high charge overpotential and poor cycle stability are the limiting factors in lithium-oxygen (Li-O 2 ) batteries, causing poor round-trip efficiency and cell failure. Many types of electrocatalysts have been explored to facilitate the oxygen evolution reaction (OER). However, even with the application of catalysts, it is still difficult to achieve stable operation as the carbon electrode (especially the defects) easily undergoes side reactions. To achieve high stability and round-trip efficiency, the rational design of OER catalysts and stable carbon electrodes are required. Herein, we employ a wet impregnation chemistry method to form a thin layer of palladium nanoparticles on the surface of carbon, which largely suppresses the side reaction through a selective coating on the carbon defect sites. Simultaneously, the Pd films serve as an electrocatalyst enabling the OER reaction with a very low overpotential. Overall, this rational design improves overall cell efficiency and extends the cycle life of the lithium-oxygen battery.

25 ENERGY STORAGE↗

Correlation between manganese dissolution and dynamic phase stability in spinel-based lithium-ion battery

Historically long accepted to be the singular root cause of capacity fading, transition metal dissolution has been reported to severely degrade the anode. However, its impact on the cathode behavior remains poorly understood. Here we show the correlation between capacity fading and phase/surface stability of an LiMn 2 O 4 cathode. It is revealed that a combination of structural transformation and transition metal dissolution dominates the cathode capacity fading. LiMn 2 O 4 exhibits irreversible phase transitions driven by manganese(III) disproportionation and Jahn-Teller distortion, which in conjunction with particle cracks results in serious manganese dissolution. Meanwhile, fast manganese dissolution in turn triggers irreversible structural evolution, and as such, forms a detrimental cycle constantly consuming active cathode components. Furthermore, lithium-rich LiMn 2 O 4 with lithium/manganese disorder and surface reconstruction could effectively suppress the irreversible phase transition and manganese dissolution. These findings close the loop of understanding capacity fading mechanisms and allow for development of longer life batteries.

25 ENERGY STORAGE↗

Silica Restricting the Sulfur Volatilization of Nickel Sulfide for High-Performance Lithium-Ion Batteries

Nickel sulfides are regarded as promising anode materials for advanced rechargeable lithium-ion batteries due to their high theoretical capacity. However, capacity fade arising from significant volume changes during operation greatly limits their practical applications. Herein, confined NiS x @C yolk-shell microboxes are constructed to address volume changes and confine the active material in the internal void space. Having benefited from the yolk-shell structure design, the prepared NiSx@C yolk-shell microboxes display excellent electrochemical performance in lithium-ion batteries. Particularly, it delivers impressive cycle stability (460 mAh g -1 after 2000 cycles at 1 A g -1 ) and superior rate performance (225 mAh g -1 at 20 A g -1 ). Furthermore, the lithium storage mechanism is ascertained with in situ synchrotron high-energy X-ray diffractions and in situ electrochemical impedance spectra. Finally, this unique confined yolk-shell structure may open up new strategies to create other advanced electrode materials for high performance electrochemical storage systems.

25 ENERGY STORAGE↗

Bamboo–Like Nitrogen–Doped Carbon Nanotube Forests as Durable Metal–Free Catalysts for Self–Powered Flexible Li–CO 2 Batteries

The Li-CO 2 battery is a promising energy storage device for wearable electronics due to its long discharge plateau, high energy density, and environmental friendliness. Furthermore, its utilization is largely hindered by poor cyclability and mechanical rigidity due to the lack of a flexible and durable catalyst electrode. Herein, flexible fiber-shaped Li-CO 2 batteries with ultralong cycle-life, high rate capability, and large specific capacity are fabricated, employing bamboo-like N-doped carbon nanotube fiber (B-NCNT) as flexible, durable metal-free catalysts for both CO 2 reduction and evolution reactions. Benefiting from high N-doping with abundant pyridinic groups, rich defects, and active sites of the periodic bamboo-like nodes, the fabricated Li-CO 2 battery shows outstanding electrochemical performance with high full-discharge capacity of 23328 mAh g -1 , high rate capability with a low potential gap up to 1.96 V at a current density of 1000 mA g -1 , stability over 360 cycles, and good flexibility. Meanwhile, the bifunctional B-NCNT is used as the counter electrode for a fiber-shaped dye-sensitized solar cell to fabricate a self-powered fiber-shaped Li-CO 2 battery with overall photochemical-electric energy conversion efficiency of up to 4.6%. Along with a stable voltage output, this design demonstrates great adaptability and application potentiality in wearable electronics with a breath monitor as an example.

25 ENERGY STORAGE↗

Exploring the charge reactions in a Li–O 2 system with lithium oxide cathodes and nonaqueous electrolytes

Nonaqueous lithium–oxygen batteries have attracted considerable attention due to their high energy density. Huge efforts have been made to unravel the fundamentals of Li–O 2 battery chemistry. However, current Li–O 2 batteries still suffer from several unresolved problems such as the instability of electrolytes and sluggish oxidation of lithium oxides during the charging process. In this paper, we propose a detailed study to investigate the charge mechanism of lithium oxide materials in different electrolytes. Commercially available lithium peroxide and lithium oxide have been employed as cathodes to determine how lithium oxides (both lithium oxide and lithium peroxide) and electrolytes change during charge. Lastly, the result shows that Li 2 O 2 decomposed to lithium and oxygen; meanwhile, the electrolyte has a significant influence on Li 2 O 2 decomposition. Furthermore, while most of the Li 2 O material participates in side reactions with the electrolyte, some of it is found to delithiate and crumble in structure.

36 MATERIALS SCIENCE↗

Commercialization of Lithium Battery Technologies for Electric Vehicles

We present that the currently commercialized lithium-ion batteries have allowed for the creation of practical electric vehicles, simultaneously satisfying many stringent milestones in energy density, lifetime, safety, power, and cost requirements of the electric vehicle economy. The next wave of consumer electric vehicles is just around the corner. Although widely adopted in the vehicle market, lithium-ion batteries still require further development to sustain their dominating roles among competitors. In this review, the authors survey the state-of-the-art active electrode materials and cell chemistries for automotive batteries. The performance, production, and cost are included. The advances and challenges in the lithium-ion battery economy from the material design to the cell and the battery packs fitting the rapid developing automotive market are discussed in detail. Additionally, new technologies of promising battery chemistries are comprehensively evaluated for their potential to satisfy the targets of future electric vehicles.

25 ENERGY STORAGE↗

In Situ Engineering of Intracellular Hemoglobin for Implantable High-Performance Biofuel Cells

The key challenge for the broad application of implantable biofuel cells (BFCs) is to achieve inorganic–organic composite biocompatibility while improving the activity and selectivity of the catalysts. We have fabricated nanoengineered red blood cells (NERBCs) by an environmentally friendly method by using red blood cells as the raw material and hemoglobin (Hb) embedded with ultrasmall hydroxyapatite (HAP, Ca 10 (PO 4 ) 6 (OH) 2 ) as the functional BFC cathode material. The NERBCs showed greatly enhanced cell performance with high electrocatalytic activity, stability, and selectivity. The NERBCs maintained the original biological properties of the natural cell, while enhancing the catalytic oxygen reduction reaction (ORR) through the interaction between -OH groups in HAP and the Hb in RBCs. Finally, they also enabled direct electron transportation, eliminating the need for an electron-transfer mediator, and showed catalytic inactivity for glucose oxidation, thus potentially enabling the development of separator-free BFCs.

09 BIOMASS FUELS↗

Electrochemically primed functional redox mediator generator from the decomposition of solid state electrolyte

Recent works into sulfide-type solid electrolyte materials have attracted much attention among the battery community. Specifically, the oxidative decomposition of phosphorus and sulfur based solid state electrolyte has been considered one of the main hurdles towards practical application. Here we demonstrate that this phenomenon can be leveraged when lithium thiophosphate is applied as an electrochemically "switched-on" functional redox mediator-generator for the activation of commercial bulk lithium sulfide at up to 70 wt.% lithium sulfide electrode content. X-ray adsorption near-edge spectroscopy coupled with electrochemical impedance spectroscopy and Raman indicate a catalytic effect of generated redox mediators on the first charge of lithium sulfide. In contrast to pre-solvated redox mediator species, this design decouples the lithium sulfide activation process from the constraints of low electrolyte content cell operation stemming from pre-solvated redox mediators. Reasonable performance is demonstrated at strict testing conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultradispersed W x C nanoparticles enable fast polysulfide interconversion for high-performance Li-S batteries

Li-S batteries are a promising next-generation battery technology but are confronted with a series of fundamental challenges, in particular the notorious shuttle effect of soluble polysulfide intermediates. Current research efforts are mostly focused on designing proper host materials for the entrapment and immobilization of polysulfides. Herein, we demonstrate that electrocatalysis may play an unexpected role in Li-S batteries. Nanosized tungsten carbide particles dispersed on the carbonaceous support are prepared from the pyrolysis of phosphotungstic acid-functionalized metal-organic frameworks. Both experimental measurements and theoretical calculations demonstrate that they not only have strong affinity toward polysulfide intermediates, but also significantly accelerate the reduction of low-order polysulfides that is otherwise kinetically challenged. Furthermore, using these supported tungsten carbide nanoparticles as the cathode catalyst, our Li-S batteries achieve large capacity, excellent cycling stability and impressive rate capability.

25 ENERGY STORAGE↗

Bridging the academic and industrial metrics for next-generation practical batteries

Batteries have shaped the modern world to an extent far beyond that of other technologies. This success is the result of the intense collaboration between Academia and Industry that took shape in the past several decades culminating with the advent and improvements of rechargeable Li-ion batteries. However, as applications are getting more demanding, stunted growth in the performance of commercial batteries risks to slow down the adoption of important technologies, such as electric vehicles. Yet, the scientific literature is full of reports describing material designs with allegedly superior performances. A large gap needs to be filled if we wish these lab-based achievements reach commercialization. In this Perspective we discuss some of the most relevant testing parameters that are often overlooked in academic literature, but that are critical for the practical applicability of lab-scale research. Metrics, such as anode energy density, voltage hysteresis, mass of the non-active cell components and anode/cathode mass ratio, will be explained and recommendation for future reporting will be made at the end of each section. We hope that this Perspective, together with other similar guiding principles that have recently started to emerge, will aid the transition from lab-scale research to next-generation practical batteries

Cao, Yuliang↗

Heteroatom-Doped Porous Carbon Materials with Unprecedented High Volumetric Capacitive Performance

The design of carbon-based materials with a high mass density and large porosity has always been a challenging goal, since they fulfill the demands of next-generation supercapacitors and other electrochemical devices. We report a new class of high-density heteroatom-doped porous carbon that can be used as an aqueous-based supercapacitor material. The material was synthesized by an in situ dehalogenation reaction between a halogenated conjugated diene and nitrogen-containing nucleophiles. Under the given conditions, pyridinium salts can only continue to perform the dehalogenation if there is residue water remaining from the starting materials. The obtained carbon materials are highly doped by various heteroatoms, leading to high densities, abundant multimodal pores, and an excellent volumetric capacitive performance. Porous carbon tri-doped with nitrogen, phosphorous, and oxygen exhibits a high packing density (2.13 g cm -3 ) and an exceptional volumetric energy density (36.8 Wh L -1 ) in alkaline electrolytes, making it competitive to even some Ni-MH cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrochemically activated spinel manganese oxide for rechargeable aqueous aluminum battery

Aluminum is a naturally abundant, trivalent charge carrier with high theoretical specific capacity and volumetric energy density, rendering aluminum-ion batteries a technology of choice for future large-scale energy storage. Nonetheless, the frequent collapse of the host structure of the cathode materials and sluggish kinetics of aluminum ion diffusion have thus far hampered the realization of practical battery devices. Here, we synthesize Al x MnO 2 •nH 2 O by an in-situ electrochemical transformation reaction to be used as a cathode material for an aluminum-ion battery with a configuration of Al/Al(OTF) 3- H 2 O/Al x MnO 2 •nH 2 O. This cell is not only based on aqueous electrolyte chemistry but also delivers a high specific capacity of 467 mAh g -1 and a record high energy density of 481 Wh kg -1 . The high safety of aqueous electrolyte, facile cell assembly and the low cost of materials suggest that this aqueous aluminum-ion battery holds promise for large-scale energy applications.

25 ENERGY STORAGE↗