Effects of carbonization temperature and time on the characteristics of carbonized sludge.

To investigate the influence of carbonization process parameters on the characteristics of municipal sludge carbonization products, this study selected carbonization temperatures of 300-700 °C and carbonization times of 0.5-1.5 h to carbonize municipal sludge. The results showed that with an increase in temperature and carbonization time, the sludge was carbonized more completely, and the structure and performance characteristics of the sludge changed significantly. Organic matter was continuously cracked, the amorphous nature of the material was reduced, its morphology was transformed into an increasing number of regular crystalline structures, and the content of carbon continued to decrease, from the initial 52.85 to 38.77%, while the content of inorganic species consisting continued to increase. The conductivity was reduced by 87.8%, and the degree of conversion of salt ions into their residual and insoluble states was significant. Natural water absorption in the sludge decreased from 8.13 to 1.29%, and hydrophobicity increased. The dry-basis higher calorific value decreased from 8,703 to 3,574 kJ/kg. Heavy metals were concentrated by a factor of 2-3, but the content of the available state was very low. The results of this study provide important technological support for the selection of suitable carbonization process conditions and for resource utilization.

Native Amino Group Directed Meta-Selective C-H Arylation of Primary Amines Via Pd/Norbornene Catalysis.

The selective functionalization of remote C-H bonds in free primary amines holds significant promise for the late-stage diversification of pharmaceuticals. However, to date, the direct functionalization of the meta position of amine substrates lacking additional directing groups remains underexplored. In this Letter, we present a successful meta-C-H arylation of free primary amine derivatives using aryl iodides, resulting in synthetically valuable yields. This meta-selective C-H functionalization is achieved through a sequence involving native amino-directed Pd-catalyzed seven-membered cyclometalation, followed by the utilization of a norbornene-type transient mediator.

Interrogations of single-cell RNA splicing landscapes with SCASL define new cell identities with physiological relevance.

RNA splicing shapes the gene regulatory programs that underlie various physiological and disease processes. Here, we present the SCASL (single-cell clustering based on alternative splicing landscapes) method for interrogating the heterogeneity of RNA splicing with single-cell RNA-seq data. SCASL resolves the issue of biased and sparse data coverage on single-cell RNA splicing and provides a new scheme for classifications of cell identities. With previously published datasets as examples, SCASL identifies new cell clusters indicating potentially precancerous and early-tumor stages in triple-negative breast cancer, illustrates cell lineages of embryonic liver development, and provides fine clusters of highly heterogeneous tumor-associated CD4 and CD8 T cells with functional and physiological relevance. Most of these findings are not readily available via conventional cell clustering based on single-cell gene expression data. Our study shows the potential of SCASL in revealing the intrinsic RNA splicing heterogeneity and generating biological insights into the dynamic and functional cell landscapes in complex tissues.

Shaping immune landscape of colorectal cancer by cholesterol metabolites.

Cancer immunotherapies have achieved unprecedented success in clinic, but they remain largely ineffective in some major types of cancer, such as colorectal cancer with microsatellite stability (MSS CRC). It is therefore important to study tumor microenvironment of resistant cancers for developing new intervention strategies. In this study, we identify a metabolic cue that determines the unique immune landscape of MSS CRC. Through secretion of distal cholesterol precursors, which directly activate RORγt, MSS CRC cells can polarize T cells toward Th17 cells that have well-characterized pro-tumor functions in colorectal cancer. Analysis of large human cancer cohorts revealed an asynchronous pattern of the cholesterol biosynthesis in MSS CRC, which is responsible for the abnormal accumulation of distal cholesterol precursors. Inhibiting the cholesterol biosynthesis enzyme Cyp51, by pharmacological or genetic interventions, reduced the levels of intratumoral distal cholesterol precursors and suppressed tumor progression through a Th17-modulation mechanism in preclinical MSS CRC models. Our study therefore reveals a novel mechanism of cancer-immune interaction and an intervention strategy for the difficult-to-treat MSS CRC.

Spatial transcriptomics deconvolution at single-cell resolution using Redeconve.

Computational deconvolution with single-cell RNA sequencing data as reference is pivotal to interpreting spatial transcriptomics data, but the current methods are limited to cell-type resolution. Here we present Redeconve, an algorithm to deconvolute spatial transcriptomics data at single-cell resolution, enabling interpretation of spatial transcriptomics data with thousands of nuanced cell states. We benchmark Redeconve with the state-of-the-art algorithms on diverse spatial transcriptomics platforms and datasets and demonstrate the superiority of Redeconve in terms of accuracy, resolution, robustness, and speed. Application to a human pancreatic cancer dataset reveals cancer-clone-specific T cell infiltration, and application to lymph node samples identifies differential cytotoxic T cells between IgA+ and IgG+ spots, providing novel insights into tumor immunology and the regulatory mechanisms underlying antibody class switch.

Bio-inspired optical structures for enhancing luminescence.

Luminescence is an essential signal for many plants, insects, and marine organisms to attract the opposite sex, avoid predators, and so on. Most luminescent living organisms have ingenious optical structures which can help them get high luminescent performances. These remarkable and efficient structures have been formed by natural selection from long-time evolution. Researchers keenly observed the enhanced luminescence phenomena and studied how these phenomena happen in order to learn the characteristics of bio-photonics. In this review, we summarize the optical structures for enhancing luminescence and their applications. The structures are classified according to their different functions. We focus on how researchers use these biological inspirations to enhance different luminescence processes, such as chemiluminescence (CL), photoluminescence (PL), and electroluminescence (EL). It lays a foundation for further research on the applications of luminescence enhancement. Furthermore, we give examples of luminescence enhancement by bio-inspired structures in information encryption, biochemical detection, and light sources. These examples show that it is possible to use bio-inspired optical structures to solve complex problems in optical applications. Our work will provide guidance for research on biomimetic optics, micro- and nano-optical structures, and enhanced luminescence.

Criteria for Efficient Photocatalytic Water Splitting Revealed by Studying Carrier Dynamics in a Model Al-doped SrTiO3 Photocatalyst.

Overall water splitting (OWS) using semiconductor photocatalysts is a promising method for solar fuel production. Achieving a high quantum efficiency is one of the most important prerequisites for photocatalysts to realize high solar-to-fuel efficiency. In a recent study (Nature 2020, 58, 411-414), a quantum efficiency of almost 100 % has been achieved in an aluminum-doped strontium titanate (SrTiO3 : Al) photocatalyst. Herein, using the SrTiO3 : Al as a model photocatalyst, we reveal the criteria for efficient photocatalytic water splitting by investigating the carrier dynamics through a comprehensive photoluminescence study. It is found that the Al doping suppresses the generation of Ti3+ recombination centers in SrTiO3 , the surface band bending facilitates charge separation, and the in situ photo-deposited Rh/Cr2 O3 and CoOOH co-catalysts render efficient charge extraction. By suppressing photocarrier recombination and establishing a facile charge separation and extraction mechanism, high quantum efficiency can be achieved even on photocatalysts with a very short (sub-ns) intrinsic photocarrier lifetime, challenging the belief that a long carrier lifetime is a fundamental requirement. Our findings could provide guidance on the design of OWS photocatalysts toward more efficient solar-to-fuel conversion.

Effect of steric hindrance and number of substituents on the transfer and interface properties of Y-shaped hole-transporting materials for perovskite solar cells.

Alkyl sulfoxide groups were introduced into the branch chain terminals of a hole-transporting material (HTM) Z34 with different numbers and positions to design four new Y-shaped HTMs: ZT1, ZT2, ZT3 and ZT4. The effects of steric hindrance and number of substituents on the transfer and interface properties of the Y-shaped HTMs were investigated theoretically. Calculations reveal that the introduction of alkyl sulfoxide increases the distribution of intramolecular holes and orbital overlap between the HOMOs of the dimers. The electronic coupling was greatly improved owing to the increased distribution of holes and orbital overlap. ZT1 shows small steric hindrance when one alkyl sulfoxide is introduced into the top branch chain, which leads to translation π-π stacking. ZT2 and ZT4 show slightly greater steric hindrance when two or four alkyl sulfoxide groups are introduced into the side branch chains, which leads to face-to-face stacking. While ZT3 shows large steric hindrance when three alkyl sulfoxide groups are introduced into the top and side branch chains, which causes head-to-head stacking. With the increase in number of alkyl sulfoxide groups, the steric hindrance of the molecule increases and the hole mobility decreases. ZT1 achieves the highest hole mobility (2.63 × 10-2 m2 V-1 s-1) that is two orders of magnitude higher than that of Z34 (1.36 × 10-4 m2 V-1 s-1) owing to the optimal balance between the number of alkyl sulfoxide groups and steric hindrance. The HTM/CH3NH3PbI3 adsorbed system was also simulated to characterize the interface properties. Enhanced interface interaction was achieved in the HTM/perovskite systems of ZT2 and ZT3. The orbital distribution of the HTM/perovskite cluster indicates that the new HTMs can promote hole migration and prevent internal electron-hole recombination. The present work not only evaluates the reliable relationship between the structure and properties of new HTMs, but also provides a valuable design strategy for efficient Y-shaped HTMs.

Decoding Human Biology and Disease Using Single-cell Omics Technologies.

Over the past decade, advances in single-cell omics (SCO) technologies have enabled the investigation of cellular heterogeneity at an unprecedented resolution and scale, opening a new avenue for understanding human biology and disease. In this review, we summarize the developments of sequencing-based SCO technologies and computational methods, and focus on considerable insights acquired from SCO sequencing studies to understand normal and diseased properties, with a particular emphasis on cancer research. We also discuss the technological improvements of SCO and its possible contribution to fundamental research of the human, as well as its great potential in clinical diagnoses and personalized therapies of human disease.

A pan-cancer single-cell panorama of human natural killer cells.

Natural killer (NK) cells play indispensable roles in innate immune responses against tumor progression. To depict their phenotypic and functional diversities in the tumor microenvironment, we perform integrative single-cell RNA sequencing analyses on NK cells from 716 patients with cancer, covering 24 cancer types. We observed heterogeneity in NK cell composition in a tumor-type-specific manner. Notably, we have identified a group of tumor-associated NK cells that are enriched in tumors, show impaired anti-tumor functions, and are associated with unfavorable prognosis and resistance to immunotherapy. Specific myeloid cell subpopulations, in particular LAMP3+ dendritic cells, appear to mediate the regulation of NK cell anti-tumor immunity. Our study provides insights into NK-cell-based cancer immunity and highlights potential clinical utilities of NK cell subsets as therapeutic targets.

Single-cell analyses implicate ascites in remodeling the ecosystems of primary and metastatic tumors in ovarian cancer.

Ovarian cancer (OC) is an aggressive gynecological tumor usually diagnosed with widespread metastases and ascites. Here, we depicted a single-cell landscape of the OC ecosystem with five tumor-relevant sites, including omentum metastasis and malignant ascites. Our data reveal the potential roles of ascites-enriched memory T cells as a pool for tumor-infiltrating exhausted CD8+ T cells and T helper 1-like cells. Moreover, tumor-enriched macrophages exhibited a preference for monocyte-derived ontogeny, whereas macrophages in ascites were more of embryonic origin. Furthermore, we characterized MAIT and dendritic cells in malignant ascites, as well as two endothelial subsets in primary tumors as predictive biomarkers for platinum-based chemotherapy response. Taken together, our study provides a global view of the female malignant ascites ecosystem and offers valuable insights for its connection with tumor tissues and paves the way for potential markers of efficacy evaluation and therapy resistance in OC.

Perovskite single-crystal thin films: preparation, surface engineering, and application.

Perovskite single-crystal thin films (SCTFs) have emerged as a significant research hotspot in the field of optoelectronic devices owing to their low defect state density, long carrier diffusion length, and high environmental stability. However, the large-area and high-throughput preparation of perovskite SCTFs is limited by significant challenges in terms of reducing surface defects and manufacturing high-performance devices. This review focuses on the advances in the development of perovskite SCTFs with a large area, controlled thickness, and high quality. First, we provide an in-depth analysis of the mechanism and key factors that affect the nucleation and crystallization process and then classify the methods of preparing perovskite SCTFs. Second, the research progress on surface engineering for perovskite SCTFs is introduced. Third, we summarize the applications of perovskite SCTFs in photovoltaics, photodetectors, light-emitting devices, artificial synapse and field-effect transistor. Finally, the development opportunities and challenges in commercializing perovskite SCTFs are discussed.

Accelerating the understanding of cancer biology through the lens of genomics.

A core mission of cancer genomics is to comprehensively chart molecular underpinnings of cancer-driving events and to provide personalized therapeutic strategies. Primarily focused on cancer cells, cancer genomics studies have successfully uncovered many drivers for major cancer types. Since the emergence of cancer immune evasion as a critical cancer hallmark, the paradigm has been elevated to the holistic tumor ecosystem, with distinct cellular components and their functional states elucidated. We highlight the milestones of cancer genomics, depict the evolving path of the field, and discuss future directions in completing the understanding of the tumor ecosystem and in advancing therapeutic strategies.

Precise Control of Crystallization and Phase-Transition with Green Anti-Solvent in Wide-Bandgap Perovskite Solar Cells with Open-Circuit Voltage Exceeding 1.25 V.

Wide-bandgap perovskite solar cells (PSCs) have attracted a lot of attention due to their application in tandem solar cells. However, the open-circuit voltage (VOC ) of wide-bandgap PSCs is dramatically limited by high defect density existing at the interface and bulk of the perovskite film. Here, an anti-solvent optimized adduct to control perovskite crystallization strategy that reduces nonradiative recombination and minimizes VOC deficit is proposed. Specifically, an organic solvent with similar dipole moment, isopropanol (IPA) is added into ethyl acetate (EA) anti-solvent, which is beneficial to form PbI2 adducts with better crystalline orientation and direct formation of α-phase perovskite. As a result, EA-IPA (7-1) based 1.67 eV PSCs deliver a power conversion efficiency of 20.06% and a VOC of 1.255 V, which is one of the remarkable values for wide-bandgap around 1.67 eV. The findings provide an effective strategy for controlling crystallization to reduce defect density in PSCs.

Spatiotemporal Changes in Frost-Free Season and Its Influence on Spring Wheat Potential Yield on the Qinghai-Tibet Plateau from 1978 to 2017.

Accurately assessing the variation in the frost-free season (FFS) can provide decision support for improving agricultural adaptability and reducing frost harm; however, related studies were inadequate in terms of the Qinghai-Tibet Plateau (QTP). This study analyzed the spatiotemporal changes in the first frost day in autumn (FFA), last frost day in spring (LFS), FFS length and effective accumulated temperature (EAT) during the 1978-2017 period, and their influences on spring wheat potential yield on the QTP, based on daily climatic data and the methodology of Sen's slope and correlation analysis. The results showed that the annual average FFA and LFS occurred later and earlier from northwest to southeast, respectively, and both the FFS length and EAT increased. From 1978 to 2017, the average regional FFA and LFS were delayed and advanced at rates of 2.2 and 3.4 days per decade, and the FFS and EAT increased by 5.6 days and 102.7 °C·d per decade, respectively. Spatially, the increase rate of FFS length ranged from 2.8 to 11.2 days per decade throughout the QTP, and it was observed to be larger in northern Qinghai, central Tibet and Yunnan, and smaller mainly in eastern Sichuan and southern Tibet. Correspondingly, the increase rate for EAT ranged from 16.2 to 173.3 °C·d per decade and generally showed a downward trend from north to south. For a one-day increase in the FFS period, the spring wheat potential yield would decrease by 17.4 and 9.0 kg/ha in altitude ranges of <2000 m and 2000-3000 m, but decrease by 24.9 and 66.5 kg/ha in the ranges of 3000-4000 m and >4000 m, respectively. Future studies should be focused on exploring the influence of multiple climatic factors on crop production using experimental field data and model technologies to provide policy suggestions.

Large-Area Black Phosphorus/PtSe2 Schottky Junction for High Operating Temperature Broadband Photodetectors.

High operating temperature (HOT) broadband photodetectors are urgently necessary for extreme condition applications in infrared-guided missiles, infrared night vision, fire safety imaging, and space exploration sensing. However, conventional photodetectors show dramatic carrier mobility decreases and carrier losses with low photoresponsivity at HOT due to the increased carrier scattering in channels at high temperatures. Herein, the HOT broadband photodetectors from room temperature to 470 K are developed for the first time by large-area black phosphorus (BP)/PtSe2 films device arrays via a depletion-enhanced photocarrier dynamics strategy. Attributed to the 2D Schottky junction at BP/PtSe2 interface and resulting in full depleted working channels, the BP/PtSe2 photodetector arrays exhibit high tolerance to carrier mobility decrease during the increasing operating temperature in a wide wavelength range from 532 to 2200 nm. Thus, the photodetector shows a state-of-the-art operating temperature at 470 K with the photo-responsivity (R) and specific detectivity (D*) of 25 A W-1 and 6.4 × 1011 Jones under 1850 nm illumination, respectively. Moreover, BP/PtSe2 photodetector arrays show high-uniformity photo-response in a large area. This work provides new strategies for high-performance broadband photodetector arrays with HOT by Schottky junction of large-area BP/PtSe2 films.

Native Amino Group Directed Site-Selective ε-C(sp2)-H Iodination of Primary Amines.

Selective remote C-H activating amines using unmodified NH2 as a native directing group demonstrate compelling synthetic utilities. The 3-arylpropan-1-amine moiety is present in many drugs and candidates in clinical trials. Selective iodination of 3-arylpropan-1-amines on remote aryl rings gives valuable intermediates for modifying bioactive molecules and synthesizing quinolones. Here we report the first palladium-catalyzed selective ε-C(sp2)-H iodination of free 3-arylpropan-1-amines via a seven-membered palladacycle.