Abstract Context The need for children's palliative care (CPC) globally is unknown. In order to understand the scope of the need and to advocate to meet it, more accurate estimates are needed. ...Objectives To create an accurate global estimate of the worldwide need for CPC based on a representative sample of countries from all regions of the world and all World Bank income groups. Methods This work builds on previously published methods developed by the International Children's Palliative Care Network, UNICEF, and WHO and tested in three African countries. The study used a cross-sectional design with quantitative data obtained from primary and secondary data sources. Estimation of the need used prevalence data from the Institute for Health Metrics and Evaluation, mortality data from the WHO for the specific diseases known to require CPC, and UNAIDS data on HIV prevalence. Representative data were analyzed for twenty-three countries representing 59.5% of the world's population. Results The findings show estimated need for children's palliative care ranged from almost 120 per 10,000 children in Zimbabwe to slightly more than 20 per 10,000 in the United Kingdom. Overall, among the over 21 million with conditions that will benefit annually from a palliative care approach, more than 8 million need specialized children's palliative care worldwide. Conclusion The estimation of need for CPC is a critical step in meeting the needs of children with life-threatening conditions and provides a sound platform to advocate for closure of the unacceptably wide gaps in coverage.
In an age of rapid acceleration toward next-generation energy storage technologies, lithium–sulfur (Li–S) batteries offer the desirable combination of low weight and high specific energy. ...Metal–organic frameworks (MOFs) have been recently studied as functionalizable platforms to improve Li–S battery performance. However, many MOF-enabled Li–S technologies are hindered by low capacity retention and poor long-term performance due to low electronic conductivity. In this work, we combine the advantages of a Zr-based MOF-808 loaded with sulfur as the active material with a graphene/ethyl cellulose additive, leading to a high-density nanocomposite electrode requiring minimal carbon. Our electrochemical results indicate that the nanocomposites deliver enhanced specific capacity over conventionally used carbon/binder mixtures, and postsynthetic modification of the MOF with lithium thiophosphate results in further improvement. Furthermore, the dense form factor of the sulfur-loaded MOF–graphene nanocomposite electrodes provides high volumetric capacity compared to other works with significantly more carbon additives. Overall, we have demonstrated a proof-of-concept paradigm where graphene nanosheets facilitate improved charge transport because of enhanced interfacial contact with the active material. This materials engineering approach can likely be extended to other MOF systems, contributing to an emerging class of two-dimensional nanomaterial-enabled Li–S batteries.
Solid-state electrolytes based on ionic liquids and a gelling matrix are promising for rechargeable lithium-ion batteries due to their safety under diverse operating conditions, favorable ...electrochemical and thermal properties, and wide processing compatibility. However, gel electrolytes also suffer from low mechanical moduli, which imply poor structural integrity and thus an enhanced probability of electrical shorting, particularly under conditions that are favorable for lithium dendrite growth. Here, we realize high-modulus, ion-conductive gel electrolytes based on imidazolium ionic liquids and exfoliated hexagonal boron nitride (hBN) nanoplatelets. Compared to conventional bulk hBN microparticles, exfoliated hBN nanoplatelets improve the mechanical properties of gel electrolytes by 2 orders of magnitude (shear storage modulus ∼5 MPa), while retaining high ionic conductivity at room temperature (>1 mS cm–1). Moreover, exfoliated hBN nanoplatelets are compatible with high-voltage cathodes (>5 V vs Li/Li+) and impart exceptional thermal stability that allows high-rate operation of solid-state rechargeable lithium-ion batteries at temperatures up to 175 °C.
LiNiO2 (LNO) is a promising cathode material for next‐generation Li‐ion batteries due to its exceptionally high capacity and cobalt‐free composition that enables more sustainable and ethical ...large‐scale manufacturing. However, its poor cycle life at high operating voltages over 4.1 V impedes its practical use, thus motivating efforts to elucidate and mitigate LiNiO2 degradation mechanisms at high states of charge. Here, a multiscale exploration of high‐voltage degradation cascades associated with oxygen stacking chemistry in cobalt‐free LiNiO2, is presented. Lattice oxygen loss is found to play a critical role in the local O3–O1 stacking transition at high states of charge, which subsequently leads to Ni‐ion migration and irreversible stacking faults during cycling. This undesirable atomic‐scale structural evolution accelerates microscale electrochemical creep, cracking, and even bending of layers, ultimately resulting in macroscopic mechanical degradation of LNO particles. By employing a graphene‐based hermetic surface coating, oxygen loss is attenuated in LNO at high states of charge, which suppresses the initiation of the degradation cascade and thus substantially improves the high‐voltage capacity retention of LNO. Overall, this study provides mechanistic insight into the high‐voltage degradation of LNO, which will inform ongoing efforts to employ cobalt‐free cathodes in Li‐ion battery technology.
Lattice oxygen loss is found to play a critical role in the O3–O1 stacking transition in cobalt‐free LiNiO2 lithium‐ion battery cathodes, which subsequently induces Ni‐ion migration and irreversible stacking faults, microscale creep, cracking, and even bending of layers after high‐voltage cycling. By suppressing oxygen evolution, hermetic graphene coatings arrest this degradation cascade, resulting in substantially improved high‐voltage capacity retention.
Aerosol jet printing is a noncontact, digital, additive manufacturing technique compatible with a wide variety of functional materials. Although promising, development of new materials and devices ...using this technique remains hindered by limited rational ink formulation, with most recent studies focused on device demonstration rather than foundational process science. In the present work, a systematic approach to formulating a polymer-stabilized graphene ink is reported, which considers the effect of solvent composition on dispersion, rheology, wetting, drying, and phase separation characteristics that drive process outcomes. It was found that a four-component solvent mixture composed of isobutyl acetate, diglyme, dihydrolevoglucosenone, and glycerol supported efficient ink atomization and controlled in-line drying to reduce overspray and wetting instabilities while maintaining high resolution and electrical conductivity, thus overcoming a trade-off in deposition rate and resolution common to aerosol jet printing. Biochemical sensors were printed for amperometric detection of the pesticide parathion, exhibiting a detection limit of 732 nM and a sensitivity of 34 nA μM–1, demonstrating the viability of this graphene ink for fabricating functional electronic devices.
Printed 2D materials, derived from solution‐processed inks, offer scalable and cost‐effective routes to mechanically flexible optoelectronics. With micrometer‐scale control and broad processing ...latitude, aerosol‐jet printing (AJP) is of particular interest for all‐printed circuits and systems. Here, AJP is utilized to achieve ultrahigh‐responsivity photodetectors consisting of well‐aligned, percolating networks of semiconducting MoS2 nanosheets and graphene electrodes on flexible polyimide substrates. Ultrathin (≈1.2 nm thick) and high‐aspect‐ratio (≈1 μm lateral size) MoS2 nanosheets are obtained by electrochemical intercalation followed by megasonic atomization during AJP, which not only aerosolizes the inks but also further exfoliates the nanosheets. The incorporation of the high‐boiling‐point solvent terpineol into the MoS2 ink is critical for achieving a highly aligned and flat thin‐film morphology following AJP as confirmed by grazing‐incidence wide‐angle X‐ray scattering and atomic force microscopy. Following AJP, curing is achieved with photonic annealing, which yields quasi‐ohmic contacts and photoactive channels with responsivities exceeding 103 A W−1 that outperform previously reported all‐printed visible‐light photodetectors by over three orders of magnitude. Megasonic exfoliation coupled with properly designed AJP ink formulations enables the superlative optoelectronic properties of ultrathin MoS2 nanosheets to be preserved and exploited for the scalable additive manufacturing of mechanically flexible optoelectronics.
Fully aerosol‐jet printed (AJP) photodetectors are fabricated using megasonically exfoliated MoS2 channels and graphene electrodes. Superlative optoelectronic performance is attributed to the megasonically thinned MoS2 nanosheets, resulting in responsivities that exceed previous all‐printed visible photodetectors by over three orders of magnitude.
Background:
Outcome measurement plays an increasing role in improving the quality, effectiveness, efficiency and availability of palliative care.
Aim:
To provide expert recommendations on outcome ...measurement in palliative care in clinical practice and research.
Methods:
Developed by a European Association for Palliative Care Task Force, based on literature searches, international expert workshop, development of outcome measurement guidance and international online survey. A subgroup drafted a first version and circulated it twice to the task force. The preliminary final version was circulated to wider expert panel and 28 international experts across 20 European Association for Palliative Care member associations and the European Association for Palliative Care Board of Directors and revised according to their feedback. The final version was approved by the European Association for Palliative Care Board for adoption as an official European Association for Palliative Care position paper.
Results:
In all, 12 recommendations are proposed covering key parameters of measures, adequate measures for the task, introduction of outcome measurement into practice, and national and international outcome comparisons and benchmarking. Compared to other recommendations, the White Paper covers similar aspects but focuses more on outcome measurement in clinical care and the wider policy impact of implementing outcome measurement in clinical palliative care. Patient-reported outcome measure feedback improves awareness of unmet need and allows professionals to act to address patients’ needs. However, barriers and facilitators have been identified when implementing outcome measurement in clinical care that should be addressed.
Conclusion:
The White Paper recommends the introduction of outcome measurement into practice and outcomes that allow for national and international comparisons. Outcome measurement is key to understanding different models of care across countries and, ultimately, patient outcome having controlled for differing patients characteristics.
Chemical sensors based on solution‐processed 2D nanomaterials represent an extremely attractive approach toward scalable and low‐cost devices. Through the implementation of real‐time impedance ...spectroscopy and development of a three‐element circuit model, redox exfoliated MoS2 nanoflakes demonstrate an ultrasensitive empirical detection limit of NO2 gas at 1 ppb, with an extrapolated ultimate detection limit approaching 63 ppt. This sensor construct reveals a more than three orders of magnitude improvement from conventional direct current sensing approaches as the traditionally dominant interflake interactions are bypassed in favor of selectively extracting intraflake doping effects. This same approach allows for an all solution‐processed, flexible 2D sensor to be fabricated on a polyimide substrate using a combination of graphene contacts and drop‐casted MoS2 nanoflakes, exhibiting similar sensitivity limits. Finally, a thermal annealing strategy is used to explore the tunability of the nanoflake interactions and subsequent circuit model fit, with a demonstrated sensitivity improvement of 2× with thermal annealing at 200 °C.
The implementation of a real‐time impedance spectroscopy approach results in ultrasensitive molecular sensors based on solution processed 2D nanomaterials. Through bypassing traditionally dominant interflake interactions and selectively extracting intraflake doping effects, detection of NO2 down to 1 ppb is readily achievable with an ultimate limit of detection of 63 ppt.
Carbon‐supported Pt nanoparticles are the leading catalysts for the cathode oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells. However, these ORR catalysts suffer from poor ...electrochemical durability, particularly the loss of electrochemical surface area (ECSA) due to Pt nanoparticle dissolution and agglomeration. Here, Pt loss is mitigated through a Pickering emulsion‐processing strategy that employs graphene nanoplatelet dispersions stabilized by the polymer ethyl cellulose. The resulting graphene‐Pt/Vulcan carbon (Pt/C) catalysts exhibit superior durability and ECSA retention throughout an accelerated stress test compared with a commercial Pt/C standard catalyst, both in a diagnostic‐rotating disc electrode setup and in a membrane electrode assembly full cell. These graphene‐Pt/C catalysts also improve durability at high‐voltage conditions, providing further evidence of their exceptional electrochemical stability. Consistent with density functional theory calculations, postelectrochemical characterization reveals that Pt nanoparticles localize at graphene defects both on the basal plane and especially at the edges of the graphene nanoplatelets. Since this Pt nanoparticle localization suppresses Pt nanoparticle dissolution and agglomeration without hindering accessibility of the reactant species to the catalyst surface, the ORR performance under both idealized and practical experimental conditions shows significantly improved durability while maintaining high electrochemical activity.
This study mitigates Pt loss for the cathode oxygen reduction reaction in polymer electrolyte membrane fuel cells through a Pickering emulsion‐processing strategy that employs graphene nanoplatelet dispersions stabilized by the polymer ethyl cellulose. The resulting catalysts exhibit superior durability and electrochemical surface area retention compared with incumbent approaches.
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