The combination of multiple-principal element materials, known as high-entropy materials (HEMs), expands the multi-dimensional compositional space to gigantic stoichiometry. It is impossible to ...afford a holistic approach to explore each possibility. With the advance of the materials genome initiative and characterization technology, a high-throughput (HT) approach is more reasonable, especially to identify the specified functions for the new HEMs development. There are three major components for the HT approach, which are the computational tools, experimental tools, and digital data. This article reviews both the materials informatics and experimental approaches for the HT methods. Applications of these tools on composition-varying samples can be used to obtain stoichiometry effectively and phase-structure-property relationships efficiently for the materials-property database establishment. They can also be used in conjunction with machine learning (ML) to improve the predictability of models. These ML tools will be an essential part of HT approaches to develop the new HEMs. The ML-developed HEMs together with ML-created other materials are positioned in this manuscript for future HEMs advancement. Comparing all the reviewed properties, the hierarchical microstructures together with the heterogeneous grain sizes show the highest potential to apply ML for new HEMs, which needs HT validations to accelerate the development. The promising potential and the database from the HEMs exploration would shed light on the future of humanity building from the scratch of Mars regolith.
Photocatalytic hydrogen evolution from natural seawater faces the severe challenges of abundant salts, which adsorb on the active sites and result in undesirable side reactions and photocatalyst ...poisoning. Herein, a series of main‐chain‐engineered discontinuously conjugated polymer (DCP) photocatalysts is presented with bifunctional crown ether (CE) structures for hydrogen evolution from seawater. The hydrophilic CE can significantly inhibit the aggregation of DCPs induced by salts. Meanwhile, cyclic CE can effectively adsorb cations to uncover the active sites to increase their interaction with protons, which can increase the hydrogen evolution rates and significantly reduce the efficiency roll‐off in natural seawater. Through atomistic studies, the formation of hydrogen bonds with bifunctional CE is elucidated and further analysis of the microscale mechanisms is also conducted using molecular dynamics and ab initio techniques. This work suggests that CE‐based polymer has the potential to enhance its ability to produce hydrogen through photocatalysis using seawater.
The first example of incorporating crown ether structure into polymer photocatalysts is demonstrated via a main‐chain‐engineering strategy. The innovative approach significantly reduces ion adsorption on the active sites, resulting in less hydrogen evolution reaction (HER) roll‐off in natural seawater. P‐8CE, in particaular, shows remarkable results with 200% and 258% higher HER than the model photocatalyst, PCzDBTO, in pure water and natural seawater, respectively.
Abstract
Photocatalytic water splitting is attracting considerable interest because it enables the conversion of solar energy into hydrogen for use as a zero-emission fuel or chemical feedstock. ...Herein, we present a universal approach for inserting hydrophilic non-conjugated segments into the main-chain of conjugated polymers to produce a series of discontinuously conjugated polymer photocatalysts. Water can effectively be brought into the interior through these hydrophilic non-conjugated segments, resulting in effective water/polymer interfaces inside the bulk discontinuously conjugated polymers in both thin-film and solution. Discontinuously conjugated polymer with 10 mol% hexaethylene glycol-based hydrophilic segments achieves an apparent quantum yield of 17.82% under 460 nm monochromatic light irradiation in solution and a hydrogen evolution rate of 16.8 mmol m
−2
h
−1
in thin-film. Molecular dynamics simulations show a trend similar to that in experiments, corroborating that main-chain engineering increases the possibility of a water/polymer interaction. By introducing non-conjugated hydrophilic segments, the effective conjugation length is not altered, allowing discontinuously conjugated polymers to remain efficient photocatalysis.
Abstract
Ambient-pressure room-temperature superconductivity is one ultimate goal of science, for it will bring worldwide revolutionary changes in all kinds of technology. Several room temperature ...and near room temperature hydride superconductors at ultra high pressure (≳100 GPa) have been predicted theoretically. In particular, the hydrogen sulfide (H
3
S) with
T
C
≃ 203 K at 200 GPa has soon been confirmed experimentally, establishing a milestone toward room temperature superconductivity. However, high-
T
C
superconductors at lower pressure (≲100 GPa) have not been reported before. In this work, we present high-
T
C
superconductivity of 180 K at a relatively low pressure of 50 GPa in sodium hydride clathrate structure NaH
6
. The
T
C
can be raised up to 206 K at 100 GPa, similar to the
T
C
of H
3
S but at a much lower pressure. At 200 GPa, it reaches the highest
T
C
of 210 K, slightly higher than that of H
3
S. The strong electron–phonon coupling strength given by the
T
2
g
phonon mode at Γ point plays the key role in superconductivity. Our work demonstrates theoretically that hydrides could stabilize at a relatively low pressure and host high-
T
C
superconductivity.
Conjugated polymers (CPs) have recently gained increasing attention as photocatalysts for sunlight-driven hydrogen evolution. However, they suffer from insufficient electron output sites and poor ...solubility in organic solvents, severely limiting their photocatalytic performance and applicability. Herein, solution-processable all-acceptor (A
-A
)-type CPs based on sulfide-oxidized ladder-type heteroarene are synthesized. A
-A
-type CPs showed upsurging efficiency improvements by two to three orders of magnitude, compared to their donor-acceptor -type CP counterparts. Furthermore, by seawater splitting, PBDTTTSOS exhibited an apparent quantum yield of 18.9% to 14.8% at 500 to 550 nm. More importantly, PBDTTTSOS achieved an excellent hydrogen evolution rate of 35.7 mmol h
g
and 150.7 mmol h
m
in the thin-film state, which is among the highest efficiencies in thin film polymer photocatalysts to date. This work provides a novel strategy for designing polymer photocatalysts with high efficiency and broad applicability.
Quantum key distribution (QKD) promises unconditional security for communication. However, the random choices of the measurement basis in QKD usually result in low key creation efficiency. This ...drawback is overcome in the differential-phase-shift QKD, provided that each photon can be prepared in a large number of time slots with a proper waveform. In this work we develop a miniature room-temperature 1550-nm single-photon source to generate narrowband single photon in 50 time slots with a nearly optimal waveform for achieving unity key creation efficiency. By utilizing these single photons in the field test, we demonstrate the differential-phase-shift QKD with a key creation efficiency of 97%. Our work shows that the practical QKD can benefit from the narrowband single photons with controllable waveforms.
Beginning with our exciting discovery of germanium (Ge) spherical quantum-dot (QD) formation via the peculiar and symbiotic interactions of Si, Ge, and O interstitials, we have embarked on a journey ...of vigorous exploration, creating unique configurations of self-organized Ge-QDs/Si-containing layers. Our aim is to generate advanced Ge-QD photonic devices, while using standard, mainstream Si processing techniques. This paper summarizes our portfolio of innovative Ge-QD configurations. With emphasis on both controllability and repeatability, we have fabricated size-tunable, spherical Ge-QDs that are placed at predetermined spatial locations within Si-containing layers (SiO
2
, Si
3
N
4
, and Si) using a coordinated combination of lithographic patterning and self-assembled growth. We have successfully exploited the multi-dimensional, parameter spaces of process conditions in combination with layout designs to achieve exquisite control available through the thermal oxidation of lithographically patterned, poly-Si
1
−
x
Ge
x
structures in close proximity with Si
3
N
4
/Si layers. In so doing, we have gained insight into the growth kinetics and formation mechanisms of self-organized, Ge spherical QDs embedded within SiO
2
, Si
3
N
4
, and Si layers, respectively. Our Ge-QD configurations have opened up a myriad of process/integration possibilities including top-to-bottom evanescent-wave coupling structures for SiN-waveguided Ge-QD photodetectors and Ge-QD light emitters for Si photonics within Si
3
N
4
integrated photonics platforms for on-chip interconnects and sensing.
There have been many clinical questions regarding whether the use of proton pump inhibitors (PPIs) could deteriorate the effects of cyclin-dependent kinase inhibitors (CDKIs) in HR+/HER2- advanced ...breast cancer patients. We performed a systematic review and meta-analysis of this clinical question, including studies enrolling HR+/HER2- metastatic breast cancer patients treated with CDKIs (Palbociclib or Ribociclib) and reporting at least one comparative survival outcome, either overall survival (OS) or progression-free survival (PFS), between concomitant PPI users and non-users. Eight studies met the eligibility criteria, with a total of 2584 patients included (PPI users: 830, PPI non-users: 1754), demonstrating that concomitant PPI use was associated with significantly higher risks of all-cause mortality (HR = 2.03; 95% CI, 1.49 to 2.77; I2 = 0%) and disease progression (HR = 1.75; 95% CI, 1.26 to 2.43; I2 = 59%) in breast cancer patients taking Palbociclib. In contrast, there were no significant survival impacts of PPIs on Ribociclib (HR = 1.46; 95% CI, 0.91 to 2.34; I2 = 36%). Additionally, there was no significant difference in the risk associated with CDKI dose reduction due to drug toxicity (RR = 1.12; 95% CI, 0.97 to 1.29). Therefore, when HR+/HER2- advanced breast cancer patients require the use of PPIs, it may be reasonable to consider using Ribociclib.
(1) Although emerging evidence suggests that proton pump inhibitor (PPI)-induced dysbiosis negatively alters treatment response to immune checkpoint inhibitors (ICIs) in cancer patients, no study ...systematically investigates the association between PPIs, ICIs, and chemotherapy; (2) Cochrane Library, Embase, Medline, and PubMed were searched from inception to 20 May 2022, to identify relevant studies involving patients receiving ICIs or chemotherapy and reporting survival outcome between PPI users and non-users. Survival outcomes included overall survival (OS) and progression-free survival (PFS). Network meta-analyses were performed using random-effects models.
-scores, with a value between 0 and 1, were calculated to quantify the treatment ranking, with a higher score suggesting a higher probability of greater effectiveness. We also conducted pairwise meta-analyses of observational studies to complement our network meta-analysis; (3) We identified 62 studies involving 26,484 patients (PPI = 8834; non-PPI = 17,650), including non-small cell lung cancer (NSCLC), urothelial carcinoma (UC), melanoma, renal cell carcinoma (RCC), hepatocellular carcinoma (HCC), and squamous cell carcinoma (SCC) of the neck and head. Eight post-hoc analyses from 18 randomized-controlled trials were included in our network, which demonstrated that, in advanced NSCLC and UC, patients under ICI treatment with concomitant PPI (
-score: 0.2016) are associated with both poorer OS (HR, 1.49; 95% CI, 1.37 to 1.67) and poorer PFS (HR, 1.41; 95% CI, 1.25 to 1.61) than those without PPIs (
-score: 1.000). Patients under ICI treatment with concomitant PPI also had poorer OS (HR, 1.18; 95% CI, 1.07 to 1.31) and poorer PFS (HR, 1.30; 95% CI, 1.14 to 1.48) in comparison with those receiving chemotherapy (
-score: 0.6664), implying that PPIs may compromise ICI's effectiveness, making it less effective than chemotherapy. Our pairwise meta-analyses also supported this association. Conversely, PPI has little effect on patients with advanced melanoma, RCC, HCC, and SCC of the neck and head who were treated with ICIs; (4) "PPI-induced dysbiosis" serves as a significant modifier of treatment response in both advanced NSCLC and UC that are treated with ICIs, compromising the effectiveness of ICIs to be less than that of chemotherapy. Thus, clinicians should avoid unnecessary PPI prescription in these patients. "PPI-induced dysbiosis", on the other hand, does not alter the treatment response to ICIs in advanced melanoma, RCC, HCC, and SCC of the head and neck.
The topological phase transition and exotic quasiparticles in materials have attracted much attention because of their potential in spintronics and mimic of elementary particles. Especially, great ...research interest has been paid to search for the Weyl fermions in solid-state physics. By using first-principles calculations, we predict that the multinary semiconductor alloy TlCd2Te4 exhibits threefold fermions and nodal-line fermions, which are protected by the S4 improper rotational symmetry. Moreover, owing to the lack of inversion and mirror symmetries, the threefold fermions split into Weyl fermions when the spin-orbit coupling is included. The chiral charge of Weyl points and the Z2 time-reversal topological invariant are investigated. The topological surface states, spin texture, and electron-phonon coupling analysis are presented. Our study demonstrates TlCd2Te4 as a good platform to understand topological phase transitions as well as possible coexistance of topological Weyl semimetal and superconductivity in one single material.
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