Tin‐based halide perovskites attract incremental attention due to the favorable optoelectronic properties and ideal bandgaps. However, the poor crystalline quality is still the biggest challenge for ...further progress in tin‐based perovskite solar cells (PVSCs) due to the unfavorable defects and uncontrollable crystallization kinetics. Here, acetic acid (HAc) is first introduced to reduce the supersaturated concentration of the precursor solution to preferentially form pre‐nucleation clusters, thus inducing rapid nucleation for effective regulation of crystallization kinetics. In particular, the hydrogen ion and acetate ion contained in HAc can effectively inhibit the oxidation of Sn2+, and the hydrogen bonding interaction between HAc and iodide ion (I‐) greatly reduces the loss of I‐, which guarantees the I‐/Sn2+ stoichiometric ratio of the corresponding perovskite film close to theoretical value, thus effectively reducing the defect density and maintaining the perfect crystal lattice. Consequently, the HAc‐assisted tin‐based PVSCs achieve a champion power conversion efficiency of 12.26% with superior open‐circuit voltage up to 0.75 V. Moreover, the unencapsulated device maintains nearly 90% of the initial PCE even after 3000 h storage in nitrogen atmosphere. This demonstrated strategy enables to prepare high‐quality tin‐based perovskite film with lower defect density and lattice distortion.
Acetic acid (HAc) is first introduced to reduce the supersaturated concentration of the precursor solution to form pre‐nucleation clusters, thus inducing rapid nucleation. In particular, the introduction of HAc can inhibit the oxidation of Sn2+ and reduce the loss of I‐. HAc‐assisted device deliver a champion efficiency of 12.26%, maintaining ≈90% of initial efficiency after storage in nitrogen over 3000 h.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Titanium metal–organic frameworks (Ti‐MOFs), as an appealing type of artificial photocatalyst, have shown great potential in the field of solar energy conversion due to their well‐studied photoredox ...activity (similar to TiO2) and good optical responsiveness of linkers, which serve as the antenna to absorb visible‐light. Although much effort has been dedicated to developing Ti‐MOFs with high photocatalytic activity, their solar energy conversion performances are still poor. Herein, we have implemented a covalent‐integration strategy to construct a series of multivariate Ti‐MOF/COF hybrid materials PdTCPP⊂PCN‐415(NH2)/TpPa (composites 1, 2, and 3), featuring excellent visible‐light utilization, a suitable band gap, and high surface area for photocatalytic H2 production. Notably, the resulting composites demonstrated remarkably enhanced visible‐light‐driven photocatalytic H2 evolution performance, especially for the composite 2 with a maximum H2 evolution rate of 13.98 mmol g−1 h−1 (turnover frequency (TOF)=227 h−1), which is much higher than that of PdTCPP⊂PCN‐415(NH2) (0.21 mmol g−1 h−1) and TpPa (6.51 mmol g−1 h−1). Our work thereby suggests a new approach to highly efficient photocatalysts for H2 evolution and beyond.
A series of covalently connected multivariate Ti‐MOF/COF hybrid materials were constructed demonstrating outstanding photocatalytic H2 evolution performance with a maximum H2 evolution rate of 13.98 mmol g−1 h−1 (TOF=227 h−1), much higher than the prototypical counterparts.
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Interfacial lattice mismatch and adverse reaction are the key issues hindering the development of nickel oxide (NiOx)‐based inverted perovskite solar cells (PVSCs). Herein, a p‐chlorobenzenesulfonic ...acid (CBSA) self‐assembled small‐molecule (SASM) is adopted to anchor NiOx and perovskite crystals to endow dual‐passivation. The chlorine terminal of SASMs can provide growth sites for perovskite, leading to interfacial strain release. Meanwhile, the sulfonic acid group from SASMs can passivate surface defects of NiOx, conducive to charge carrier extraction. In addition, the self‐assembled layer inhibits the adverse interfacial reaction by preventing NiOx contact with perovskite. Therefore, the NiOx/CBSA‐based PVSCs obtain a champion power conversion efficiency (PCE) of 21.8%. Of particular note, the unencapsulated devices can retain above 80% of their initial PCE values after storage in a nitrogen atmosphere for 3000 h, in air with a relative humidity of 50–70% for 1000 h, and heating at 85 °C for 800 h, respectively.
A p‐chlorobenzenesulfonic acid (CBSA)‐based self‐assembled layer dual‐passivation strategy is employed to effectively eliminate interfacial lattice mismatch and detrimental reactions in NiOx‐based perovskite solar cells, which achieves unencapsulated devices preserving above 80% of initial efficiencies after storing in N2 for 3000 h, in air with a relative humidity of 50–70% for 1000 h, and heating at 85 °C for 800 h, respectively.
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Osteosarcoma is the most frequent primary bone tumor with poor prognosis. Through RNA-sequencing of 100,987 individual cells from 7 primary, 2 recurrent, and 2 lung metastatic osteosarcoma lesions, ...11 major cell clusters are identified based on unbiased clustering of gene expression profiles and canonical markers. The transcriptomic properties, regulators and dynamics of osteosarcoma malignant cells together with their tumor microenvironment particularly stromal and immune cells are characterized. The transdifferentiation of malignant osteoblastic cells from malignant chondroblastic cells is revealed by analyses of inferred copy-number variation and trajectory. A proinflammatory FABP4
macrophages infiltration is noticed in lung metastatic osteosarcoma lesions. Lower osteoclasts infiltration is observed in chondroblastic, recurrent and lung metastatic osteosarcoma lesions compared to primary osteoblastic osteosarcoma lesions. Importantly, TIGIT blockade enhances the cytotoxicity effects of the primary CD3
T cells with high proportion of TIGIT
cells against osteosarcoma. These results present a single-cell atlas, explore intratumor heterogeneity, and provide potential therapeutic targets for osteosarcoma.
Abstract
The activity of Fischer–Tropsch synthesis (FTS) on metal-based nanocatalysts can be greatly promoted by the support of reducible oxides, while the role of support remains elusive. Herein, by ...varying the reduction condition to regulate the TiO
x
overlayer on Ru nanocatalysts, the reactivity of Ru/TiO
2
nanocatalysts can be differentially modulated. The activity in FTS shows a volcano-like trend with increasing reduction temperature from 200 to 600 °C. Such a variation of activity is characterized to be related to the activation of CO on the TiO
x
overlayer at Ru/TiO
2
interfaces. Further theoretical calculations suggest that the formation of reduced TiO
x
occurs facilely on the Ru surface, and it involves in the catalytic mechanism of FTS to facilitate the CO bond cleavage kinetically. This study provides a deep insight on the mechanism of TiO
x
overlayer in FTS, and offers an effective approach to tuning catalytic reactivity of metal nanocatalysts on reducible oxides.
Abstract
Single-atom catalysts (SACs) have emerged as a frontier in heterogeneous catalysis due to the well-defined active site structure and the maximized metal atom utilization. Nevertheless, the ...robustness of SACs remains a critical concern for practical applications. Herein, we report a highly active, selective and robust Ru SAC which was synthesized by pyrolysis of ruthenium acetylacetonate and N/C precursors at 900 °C in N
2
followed by treatment at 800 °C in NH
3
. The resultant Ru
1
-N
3
structure exhibits moderate capability for hydrogen activation even in excess NH
3
, which enables the effective modulation between transimination and hydrogenation activity in the reductive amination of aldehydes/ketones towards primary amines. As a consequence, it shows superior amine productivity, unrivalled resistance against CO and sulfur, and unexpectedly high stability under harsh hydrotreating conditions compared to most SACs and nanocatalysts. This SAC strategy will open an avenue towards the rational design of highly selective and robust catalysts for other demanding transformations.
Transport of Topological Semimetals Hu, Jin; Xu, Su-Yang; Ni, Ni ...
Annual review of materials research,
07/2019, Volume:
49, Issue:
1
Journal Article
Peer reviewed
Open access
Three-dimensional (3D) topological semimetals represent a new class of topological matters. The study of this family of materials has been at the frontiers of condensed matter physics, and many ...breakthroughs have been made. Several topological semimetal phases, including Dirac semimetals (DSMs), Weyl semimetals (WSMs), nodal-line semimetals (NLSMs), and triple-point semimetals, have been theoretically predicted and experimentally demonstrated. The low-energy excitation around the Dirac Weyl nodal points, nodal line, or triply degenerated nodal point can be viewed as emergent relativistic fermions. Experimental studies have shown that relativistic fermions can result in a rich variety of exotic transport properties, e.g., extremely large magnetoresistance, the chiral anomaly, and the intrinsic anomalous Hall effect. In this review, we first briefly introduce band structural characteristics of each topological semimetal phase, then review the current studies on quantum oscillations and exotic transport properties of various topological semimetals, and finally provide a perspective of this area.
Applications of fiber optic sensors to battery monitoring have been increasing due to the growing need of enhanced battery management systems with accurate state estimations. The goal of this review ...is to discuss the advancements enabling the practical implementation of battery internal parameter measurements including local temperature, strain, pressure, and refractive index for general operation, as well as the external measurements such as temperature gradients and vent gas sensing for thermal runaway imminent detection. A reasonable matching is discussed between fiber optic sensors of different range capabilities with battery systems of three levels of scales, namely electric vehicle and heavy-duty electric truck battery packs, and grid-scale battery systems. The advantages of fiber optic sensors over electrical sensors are discussed, while electrochemical stability issues of fiber-implanted batteries are critically assessed. This review also includes the estimated sensing system costs for typical fiber optic sensors and identifies the high interrogation cost as one of the limitations in their practical deployment into batteries. Finally, future perspectives are considered in the implementation of fiber optics into high-value battery applications such as grid-scale energy storage fault detection and prediction systems.
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