Abstract Electrochemical surface oxidation of carbon black Vulcan XC-72 and multiwalled carbon nanotube (MWNT) has been compared following potentiostatic treatments up to 168 h under condition simulating PEMFC cathode environment (60 °C, N2 purged 0.5 M H2SO4, and a constant potential of 0.9 V). The subsequent electrochemical characterization at different treatment time intervals suggests that MWNT is electrochemically more stable than Vulcan XC-72 with less surface oxide formation and 30% lower corrosion current under the investigated condition. As a result of high corrosion resistance, MWNT shows lower loss of Pt surface area and oxygen reduction reaction activity when used as fuel cell catalyst support.

http://ma.ecsdl.org/content/MA2005-02/33/1168.full.pdf

Durability Investigation of Carbon Nanotube as Catalyst Support for Proton Exchange Membrane Fuel Cell Electrode

Electrocatalysts with single metal atoms as active sites have received increasing attention owing to their high atomic utilization efficiency and exotic catalytic activity and selectivity. This review aims to provide a comprehensive summary on the recent development of such single-atom electrocatalysts (SAECs) for various energy-conversion reactions. The discussion starts with an introduction of the different types of SAECs, followed by an overview of the synthetic methodologies to control the atomic dispersion of metal sites and atomically resolved characterization using state-of-the-art microscopic and spectroscopic techniques. In recognition of the extensive applications of SAECs, the electrocatalytic studies are dissected in terms of various important electrochemical reactions, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO2RR), and nitrogen reduction reaction (NRR). Examples of SAECs are deliberated in each case in terms of their catalytic performance, structure-property relationships, and catalytic enhancement mechanisms. A perspective is provided at the end of each section about remaining challenges and opportunities for the development of SAECs for the targeted reaction.

Advanced Electrocatalysts with Single-Metal-Atom Active Sites.

The urgent need to address the high-cost issue of proton-exchange membrane fuel cell (PEMFC) technologies, particularly for transportation applications, drives the development of simultaneously highly active and durable platinum group metal-free (PGM-free) catalysts and electrodes. The past decade has witnessed remarkable progress in exploring PGM-free cathode catalysts for the oxygen reduction reaction (ORR) to overcome sluggish kinetics and catalyst instability in acids. Among others, scientists have identified the newly emerging atomically dispersed transition metal (M: Fe, Co, or/and Mn) and nitrogen co-doped carbon (M-N-C) catalysts as the most promising alternative to PGM catalysts. Here, we provide a comprehensive review of significant breakthroughs, remaining challenges, and perspectives regarding the M-N-C catalysts in terms of catalyst activity, stability, and membrane electrode assembly (MEA) performance. A variety of novel synthetic strategies demonstrated effectiveness in improving intrinsic activity, increasing active site density, and attaining optimal porous structures of catalysts. Rationally designing and engineering the coordination environment of single metal MNx sites and their local structures are crucial for enhancing intrinsic activity. Increasing the site density relies on the innovative strategies of restricting the migration and agglomeration of single metal sites into metallic clusters. Relevant understandings provide the correlations among the nature of active sites, nanostructures, and catalytic activity of M-N-C catalysts at the atomic scale through a combination of experimentation and theory. Current knowledge of the transferring catalytic properties of M-N-C catalysts to MEA performance is limited. Rationally designing morphologic features of M-N-C catalysts play a vital role in boosting electrode performance through exposing more accessible active sites, realizing uniform ionomer distribution, and facilitating mass/proton transports. We outline future research directions concerning the comprehensive evaluation of M-N-C catalysts in MEAs. The most considerable challenge of current M-N-C catalysts is the unsatisfied stability and rapid performance degradation in MEAs. Therefore, we further discuss practical methods and strategies to mitigate catalyst and electrode degradation, which is fundamentally essential to make M-N-C catalysts viable in PEMFC technologies.

Atomically dispersed metal–nitrogen–carbon catalysts for fuel cells: advances in catalyst design, electrode performance, and durability improvement

The development of catalysts free of platinum-group metals and with both a high activity and durability for the oxygen reduction reaction in proton exchange membrane fuel cells is a grand challenge. Here we report an atomically dispersed Co and N co-doped carbon (Co–N–C) catalyst with a high catalytic oxygen reduction reaction activity comparable to that of a similarly synthesized Fe–N–C catalyst but with a four-time enhanced durability. The Co–N–C catalyst achieved a current density of 0.022 A cm−2 at 0.9 ViR-free (internal resistance-compensated voltage) and peak power density of 0.64 W cm−2 in 1.0 bar H2/O2 fuel cells, higher than that of non-iron platinum-group-metal-free catalysts reported in the literature. Importantly, we identified two main degradation mechanisms for metal (M)–N–C catalysts: catalyst oxidation by radicals and active-site demetallation. The enhanced durability of Co–N–C relative to Fe–N–C is attributed to the lower activity of Co ions for Fenton reactions that produce radicals from the main oxygen reduction reaction by-product, H2O2, and the significantly enhanced resistance to demetallation of Co–N–C. Platinum-group-metal-free, non-iron catalysts are highly desirable for the oxygen reduction reaction at proton exchange membrane (PEM) fuel cell cathodes, as they avoid the detrimental Fenton reactions. Now, a cobalt and nitrogen co-doped carbon catalyst with atomically dispersed porphyrin-like CoN4C12 sites is reported with an improved activity and durability in PEM fuel cell conditions.

Performance enhancement and degradation mechanism identification of a single-atom Co–N–C catalyst for proton exchange membrane fuel cells

Significance Efficient thermal transport is critical for applications ranging from electronics and energy to advanced manufacturing and transportation; it is essential in emerging domains like wearable computing and soft robotics, which require thermally conductive materials that are also soft and stretchable. However, heat transport within soft materials is limited by the dynamics of phonon transport, which results in a trade-off between thermal conductivity and compliance. We overcome this by engineering an elastomer composite embedded with elongated inclusions of liquid metal (LM) that function as thermally conductive pathways. These composites exhibit an extraordinary combination of low stiffness (<100 kPa), high strain limit (>600%), and metal-like thermal conductivity (up to 9.8 W⋅m−1⋅K−1) that far exceeds any other soft materials. Soft dielectric materials typically exhibit poor heat transfer properties due to the dynamics of phonon transport, which constrain thermal conductivity (k) to decrease monotonically with decreasing elastic modulus (E). This thermal−mechanical trade-off is limiting for wearable computing, soft robotics, and other emerging applications that require materials with both high thermal conductivity and low mechanical stiffness. Here, we overcome this constraint with an electrically insulating composite that exhibits an unprecedented combination of metal-like thermal conductivity, an elastic compliance similar to soft biological tissue (Young’s modulus < 100 kPa), and the capability to undergo extreme deformations (>600% strain). By incorporating liquid metal (LM) microdroplets into a soft elastomer, we achieve a ∼25× increase in thermal conductivity (4.7 ± 0.2 W⋅m−1⋅K−1) over the base polymer (0.20 ± 0.01 W⋅m−1·K−1) under stress-free conditions and a ∼50× increase (9.8 ± 0.8 W⋅m−1·K−1) when strained. This exceptional combination of thermal and mechanical properties is enabled by a unique thermal−mechanical coupling that exploits the deformability of the LM inclusions to create thermally conductive pathways in situ. Moreover, these materials offer possibilities for passive heat exchange in stretchable electronics and bioinspired robotics, which we demonstrate through the rapid heat dissipation of an elastomer-mounted extreme high-power LED lamp and a swimming soft robot.

/pdf/high-thermal-conductivity-in-soft-elastomers-with-elongated-3wdtjxvzco.pdf

High thermal conductivity in soft elastomers with elongated liquid metal inclusions.

Stretchable high-dielectric-constant materials are crucial for electronic applications in emerging domains such as wearable computing and soft robotics. While previous efforts have shown promising materials architectures in the form of dielectric nano-/microinclusions embedded in stretchable matrices, the limited mechanical compliance of these materials significantly limits their practical application as soft energy-harvesting/storage transducers and actuators. Here, a class of liquid metal (LM)-elastomer nanocomposites is presented with elastic and dielectric properties that make them uniquely suited for applications in soft-matter engineering. In particular, the role of droplet size is examined and it is found that embedding an elastomer with a polydisperse distribution of nanoscale LM inclusions can enhance its electrical permittivity without significantly degrading its elastic compliance, stretchability, or dielectric breakdown strength. In contrast, elastomers embedded with microscale droplets exhibit similar improvements in permittivity but a dramatic reduction in breakdown strength. The unique enabling properties and practicality of LM-elastomer nanocomposites for use in soft machines and electronics is demonstrated through enhancements in performance of a dielectric elastomer actuator and energy-harvesting transducer.

A Liquid-Metal-Elastomer Nanocomposite for Stretchable Dielectric Materials.

Performance study of SAPO-34 and FAPO-34 desiccants for desiccant coated heat exchanger systems

Performance study on composite desiccant material coated fin-tube heat exchangers

Performance study of composite silica gels with different pore sizes and different impregnating hygroscopic salts

Low cost and high-performing platinum group metal-free (PGM-free) cathodes have the potential to transform the economics of polymer electrolyte fuel cell (PEFC) commercialization. Significant advan...

Leiming Hu

Papers

A Liquid-Metal-Elastomer Nanocomposite for Stretchable Dielectric Materials.

Performance study of SAPO-34 and FAPO-34 desiccants for desiccant coated heat exchanger systems

Performance study on composite desiccant material coated fin-tube heat exchangers

Performance study of composite silica gels with different pore sizes and different impregnating hygroscopic salts

High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells