Glycosaminogycans (GAGs) are involved in numerous vital functions in the human body. Mapping the GAG concentration in vivo is desirable for the diagnosis and monitoring of a number of diseases such as osteoarthritis, which affects millions of individuals. GAG loss in cartilage is typically an initiating event in osteoarthritis. Another widespread pathology related to GAG is intervertebral disk degeneration. Currently existing techniques for GAG monitoring, such as delayed gadolinium-enhanced MRI contrast (dGEMRIC), T1, and 23 Na MRI, have some practical limitations. We show that by exploiting the exchangeable protons of GAG one may directly measure the localized GAG concentration in vivo with high sensitivity and therefore obtain a powerful diagnostic MRI method.cartilage ͉ MRI ͉ osteoarthritis ͉ NOE ͉ proteoglycan
Tungsten carbide is one of the most promising electrocatalysts for the hydrogen evolution reaction, although it exhibits sluggish kinetics due to a strong tungsten-hydrogen bond. In addition, tungsten carbide’s catalytic activity toward the oxygen evolution reaction has yet to be reported. Here, we introduce a superaerophobic nitrogen-doped tungsten carbide nanoarray electrode exhibiting high stability and activity toward hydrogen evolution reaction as well as driving oxygen evolution efficiently in acid. Nitrogen-doping and nanoarray structure accelerate hydrogen gas release from the electrode, realizing a current density of −200 mA cm−2 at the potential of −190 mV vs. reversible hydrogen electrode, which manifest one of the best non-noble metal catalysts for hydrogen evolution reaction. Under acidic conditions (0.5 M sulfuric acid), water splitting catalyzed by nitrogen-doped tungsten carbide nanoarray starts from about 1.4 V, and outperforms most other water splitting catalysts.
The role of vacancy defects is demonstrated to be positive in various energy‐related processes. However, introducing vacancy defects into single‐crystalline nanostructures with given facets and studying their defect effect on electrocatalytic properties remains a great challenge. Here this study deliberately introduces oxygen defects into single‐crystalline ultrathin Co3O4 nanosheets with O‐terminated {111} facets by mild solvothermal reduction using ethylene glycol under alkaline condition. As‐prepared defect‐rich Co3O4 nanosheets show a low overpotential of 220 mV with a small Tafel slope of 49.1 mV dec−1 for the oxygen evolution reaction (OER), which is among the best Co‐based OER catalysts to date and even more active than the state‐of‐the‐art IrO2 catalyst. Such vacancy defects are formed by balancing with reducing environments under solvothermal conditions, but are surprisingly stable even after 1000 cycles of scanning under OER working conditions. Density functional theory plus U calculation attributes the enhanced performance to the oxygen vacancies and consequently exposed second‐layered Co metal sites, which leads to the lowered OER activation energy of 2.26 eV and improved electrical conductivity. This mild solvothermal reduction concept opens a new door for the understanding and future designing of advanced defect‐based electrocatalysts.
Chemistry at the cathode/electrolyte interface plays an important role for lithium-sulfur batteries in which stable cycling of the sulfur cathode requires confinement of the lithium polysulfide intermediates and their fast electrochemical conversion on the electrode surface. While many materials have been found to be effective for confining polysulfides, the underlying chemical interactions remain poorly understood. We report a new and general lithium polysulfide-binding mechanism enabled by surface oxidation layers of transition-metal phosphide and chalcogenide materials. We for the first time find that CoP nanoparticles strongly adsorb polysulfides because their natural oxidation (forming Co-O-P-like species) activates the surface Co sites for binding polysulfides via strong Co-S bonding. With a surface oxidation layer capable of confining polysulfides and an inner core suitable for conducting electrons, the CoP nanoparticles are thus a desirable candidate for stabilizing and improving the performance of sulfur cathodes in lithium-sulfur batteries. We demonstrate that sulfur electrodes that hold a high mass loading of 7 mg cm and a high areal capacity of 5.6 mAh cm can be stably cycled for 200 cycles. We further reveal that this new surface oxidation-induced polysulfide-binding scheme applies to a series of transition-metal phosphide and chalcogenide materials and can explain their stabilizing effects for lithium-sulfur batteries.
The salinity gradient between seawater and river water is a clean energy source and an alternative solution for the increasing energy demands. A membrane-based reverse electrodialysis technique is a promising strategy to convert osmotic energy to electricity. To overcome the limits of traditional membranes with low efficiency and high resistance, nanofluidic is an emerging technique to promote osmotic energy harvesting. Here, we engineer a high-performance nanofluidic device with a hybrid membrane composed of a silk nanofibril membrane and an anodic aluminum oxide membrane. The silk nanofibril membrane, as a screening layer with condensed negative surface and nanochannels, dominates the ion transport; the anodic aluminum oxide membrane, as a supporting substrate, offers tunable channels and amphoteric groups. Thus, a nanofluidic membrane with asymmetric geometry and charge polarity is established, showing low resistance, high-performance energy conversion, and long-term stability. The system paves avenues for sustainable power generation, water purification, and desalination.
We developed a novel methodology for the general synthesis of non-precious transition metal–nitrogen–carbon electrocatalysts based on formamide condensation.
The emerging heterogeneous membranes show unprecedented superiority in harvesting the osmotic energy between ionic solutions of different salinity. However, the power densities are limited by the low interfacial transport efficiency caused by a mismatch of pore alignment and insufficient coupling between channels of different dimensions. Here we demonstrate the use of three-dimensional (3D) gel interface to achieve high-performance osmotic energy conversion through hybridizing polyelectrolyte hydrogel and aramid nanofiber membrane. The ionic diode effect of the heterogeneous membrane facilitates one-way ion diffusion, and the gel layer provides a charged 3D transport network, greatly enhancing the interfacial transport efficiency. When used for harvesting the osmotic energy from the mixing of sea and river water, the heterogeneous membrane outperforms the state-of-the-art membranes, to the best of our knowledge, with power densities of 5.06 W m −2. The diversity of the polyelectrolyte and gel makes our strategy a potentially universal approach for osmotic energy conversion.
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