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Metavalent Bonding in 2D Chalcogenides: Structural Origin and Chemical Mechanisms

Angewandte Chemie 2023年第1期136卷

作者： Raagya Arora Umesh Waghmare C. N. R. Rao Theoretical Sciences Unit School of Advanced Materials Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR) Jakkur Bangalore 560 064 India Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Resources (equal) Software (equal) Validation (equal) Visualization (lead) Writing - original draft (equal) Writing - review & editing (equal) Sheikh Saqr Laboratory JNCASR Jakkur Bangalore 560 064 India New Chemistry Unit School of Advanced Materials JNCASR Jakkur Bangalore 560 064 India Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (equal) Project administration (lead) Resources (equal) Supervision (lead) Validation (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Supervision (equal) Writing - review & editing (equal)

An unusual set of anomalous functional properties of rocksalt crystals of Group IV chalcogenides were recently linked to a kind of bonding termed as metavalent bonding (MVB) which involves violation of the 8-N rule. Precise mechanisms of MVB and the relevance of lone pair of Group IV cations are still debated. With restrictions of low dimensionality on the possible atomic coordination, 2D materials provide a rich platform for exploration of MVB. Here, we present first-principles theoretical analysis of the nature of bonding in five distinct 2D lattices of Group IV chalcogenides MX (M: Sn, Pb, Ge and X: S, Se, Te), in which the natural out-of-plane expression of the lone pair versus in-plane bonding can be systematically explored. While their honeycomb lattices respecting the 8-N rule are shown to exhibit covalent bonding, their square and orthorhombic structures exhibit MVB only in-plane, with cationic lone pair activating the out-of-plane structural puckering that controls their relative stability. Anomalies in Born-effective charges, dielectric constants, Grüneisen parameters occur only in their in-plane behaviour, confirming MVB is confined strictly to 2D and originates from p-p orbital interactions. Our work opens up directions for chemical design of MVB based 2D materials and their heterostructures.

关键词： Electronic Structure Ferroelectrics Metavalent Bonding Phase Change Materials Thermoelectrics

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Highly Efficient Spatially–Temporally Synchronized Construction of Robust Li3PO4-rich Solid–Electrolyte Interphases in Aqueous Li-ion Batteries

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Angewandte Chemie 2023年第5期136卷

作者： Dr. Xiangzhen Zhu Dr. Zejing Lin Dr. Jingning Lai Dr. Tianshi Lv Ting Lin Dr. Hongyi Pan Jingnan Feng Dr. Qiyu Wang Shuai Han Prof. Renjie Chen Prof. Liquan Chen Prof. Liumin Suo Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China Yangtze River Delta Physics Research Center Co. Ltd. Changzhou Liyang 213300 China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Methodology (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Visualization (equal) Writing - review & editing (supporting) Beijing Key Laboratory of Environmental Science and Engineering School of Material Science & Engineering Beijing Institute of Technology Beijing 100081 China Contribution: Data curation (supporting) Contribution: Resources (supporting) Contribution: Funding acquisition (equal) Resources (equal) Supervision (equal) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (lead) Project administration (lead) Resources (lead) Supervision (lead) Writing - review & editing (equal)

Solid electrolyte interphase (SEI) makes the electrochemical window of aqueous electrolytes beyond the thermodynamics limitation of water. However, achieving the energetic and robust SEI is more challenging in aqueous electrolytes because the low SEI formation efficiency (SFE) only contributed from anion-reduced products, and the low SEI formation quality (SFQ) negatively impacted by the hydrogen evolution, resulting in a high Li loss to compensate for SEI formation. Herein, we propose a highly efficient strategy to construct Spatially-Temporally Synchronized (STS) robust SEI by the involvement of synergistic chemical precipitation-electrochemical reduction. In this case, a robust Li 3 PO 4 -rich SEI enables intelligent inherent growth at the active site of the hydrogen by the chemical capture of the OH − stemmed from the HER to trigger the ionization balance of dihydrogen phosphate (H 2 PO 4 − ) shift to insoluble solid Li 3 PO 4 . It is worth highlighting that the Li 3 PO 4 formation does not extra-consume lithium derived from the cathode but makes good use of the product of HER (OH − ), prompting the SEI to achieve 100 % SFE and pushing the HER potential into −1.8 V vs. Ag/AgCl. This energetic and robust SEI offers a new way to achieve anion/concentration-independent interfacial chemistry for the aqueous batteries.

关键词： Aqueous Batteries Electrochemcial Window Li3PO4 Solid-Electrolyte Interphase

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Inferring the population history of Kyrgyz in Xinjiang, Northwest China from genome-wide array genotyping

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American Journal of Biological Anthropology 2023年第4期181卷

作者： Bubibatima Halili Xiaomin Yang Rui Wang Kongyang Zhu Xiangjun Hai Chuan-Chao Wang Department of Anthropology and Ethnology Institute of Anthropology School of Sociology and Anthropology Xiamen University Xiamen China Contribution: Conceptualization (equal) Resources (lead) Xiangjun Hai State Key Laboratory of Cellular Stress Biology School of Life Sciences Xiamen University Xiamen 361102 China. Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Visualization (lead) Writing - original draft (lead) State Key Laboratory of Cellular Stress Biology School of Life Sciences Xiamen University Xiamen China Contribution: Data curation (equal) Formal analysis (equal) Key Laboratory of Environmental Ecology and Population Health in Northwest Minority Areas Northwest Minzu University Lanzhou China Xiaomin Yang and Chuan-Chao Wang Department of Anthropology and Ethnology Institute of Anthropology School of Sociology and Anthropology Xiamen University 361005 Xiamen China. Contribution: Conceptualization (equal) Resources (equal) State Key Laboratory of Marine Environmental Science Xiamen University Xiamen China Institute of Artificial Intelligence Xiamen University Xiamen China Ministry of Education Key Laboratory of Contemporary Anthropology Department of Anthropology and Human Genetics School of Life Sciences Fudan University Shanghai China Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

Objectives Xinjiang plays a vital role in the trans-Eurasian population migration, language diffusion, and culture and technology exchange. However, the underrepresentation of Xinjiang's genomes has hindered a more comprehensive understanding of Xinjiang's genetic structure and population history. Materials and Methods We collected and genotyped 70 southern Xinjiang's Kyrgyz (SXJK) individuals and combined the data with modern and ancient Eurasians published. We used allele-frequency methods, including PCA, ADMIXTURE, f -statistics, qpWave/qpAdm , ALDER, Treemix, and haplotype-shared methods including shared-IBD segments, fineSTRUCTURE, and GLOBETROTTER to unveil the fine-scale population structure and reconstruct admixture history. Results We identified genetic substructure within the SXJK population with subgroups showing different genetic affinities to West and East Eurasians. All SXJK subgroups were suggested to have close genetic relationships with surrounding Turkic-speaking groups that is, Uyghur, Kyrgyz from north Xinjiang and Tajikistan, and Chinese Kazakh, suggesting a shared ancestry among those populations. Outgroup- f 3 and symmetrical f 4 statistics showed a high genetic affinity of SXJK to present-day Tungusic, Mongolic-speaking populations and Ancient Northeast Asian (ANA) related groups. Allele sharing and haplotype sharing profiles revealed the east–west admixture pattern of SXJK. The qpAdm -based admixture models showed that SXJK derived ancestry from East Eurasian (ANA and East Asian, 42.7%–83.3%) and West Eurasian (Western Steppe herders and Central Asian, 16.7%–57.3%), the recent east–west admixture event could be traced to 1000 years ago based on ALDER and GLOBETROTTER analysis. Discussion The high genetic affinity of SXJK to present-day Tungusic and Mongolic-speaking populations and short-shared IBD segments indicated their shared common ancestry. SXJK harbored a close genetic affinity to ANA-related populations, indicating the Northeast Asia

关键词： admixture history genetic continuity genetic structure genome-wide SNP Kyrgyz

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Single-Photon-Induced Post-Ionization to Boost Ion Yields in MALDI Mass Spectrometry Imaging**

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Angewandte Chemie 2022年第34期134卷

作者： Dr. Christoph Bookmeyer Ulrich Röhling Prof. Dr. Klaus Dreisewerd Dr. Jens Soltwisch Institute of Hygiene University of Münster Robert-Koch-Str. 41 48149 Münster Germany Metabolomics Interdisciplinary Laboratory University of Tarragona Avinguda Països Catalans 26 43007 Tarragona (Spain) Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (equal) Visualization (lead) Writing - original draft (lead) Writing - review & editing (equal) Institute of Medical Physics and Biophysics University of Münster Robert-Koch-Str. 31 48149 Münster Germany Deceased (2021) Contribution: Conceptualization (supporting) Investigation (lead) Resources (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Methodology (supporting) Supervision (equal) Writing - original draft (supporting) Writing - review & editing (equal) Contribution: Conceptualization (lead) Data curation (supporting) Formal analysis (supporting) Funding acquisition (equal) Investigation (supporting) Methodology (equal) Supervision (lead) Writing - original draft (lead) Writing - review & editing (equal)

Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) is a rapidly growing method in the life sciences. However, for many analyte classes, its sensitivity is limited due to poor ionization efficiencies. To mitigate this problem, we here introduce a novel post-ionization scheme based on single-photon induced chemical ionization using pulsed RF-Kr lamps. The fine-vacuum conditions of a dual ion-funnel ion source effectively thermalize the evolving MALDI plume and enable ample gas-phase reactions. Injected chemical dopants crucially support fragment-less ionization to [ M +H] + /[ M −H] − species. Based on this interplay, numerous glycerophospho-, sphingo-, and further lipids, registered from mammalian tissue sections, were boosted by up to three orders of magnitude, similar to results obtained with laser-based post-ionization (MALDI-2). Experiments with deuterated matrix and dopant, however, indicated complex chemical ionization pathways different from MALDI-2.

关键词： Analytical Methods Lipidomics MALDI-MS Imaging Mass Spectrometry Post-Ionization

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Automated assessment of necrosis tumor ratio in colorectal cancer using an artificial intelligence-based digital pathology analysis

Medicine Advances

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Medicine Advances 2023年第1期1卷

作者： Huifen Ye Yunrui Ye Yiting Wang Tong Tong Su Yao Yao Xu Qingru Hu Yulin Liu Changhong Liang Guangyi Wang Ke Zhao Xinjuan Fan Yanfen Cui Zaiyi Liu Department of Radiology Guangdong Provincial People's Hospital (Guangdong Academy of Medical Sciences) Southern Medical University Guangzhou China The Second School of Clinical Medicine Southern Medical University Guangzhou China Guangdong Provincial Key Laboratory of Artificial Intelligence in Medical Image Analysis and Application Guangzhou China Contribution: Conceptualization (equal) Methodology (equal) Visualization (equal) Writing - original draft (equal) Contribution: Data curation (equal) Investigation (equal) Validation (equal) Writing - original draft (equal) Department of Pathology The Sixth Affiliated Hospital of Sun Yat-sen University Guangzhou China Contribution: Data curation (equal) Investigation (equal) Validation (equal) Formal analysis (equal) Department of Radiology Fudan University Shanghai Cancer Center Shanghai China Department of Oncology Shanghai Medical College Shanghai China Contribution: Data curation (equal) Investigation (equal) Validation (equal) Department of Pathology Guangdong Provincial People's Hospital (Guangdong Academy of Medical Sciences) Southern Medical University Guangzhou China Contribution: Formal analysis (equal) Contribution: Formal analysis (equal) Supervision (equal) Writing - review & editing (equal) Guangdong Cardiovascular Institute Guangdong Provincial People's Hospital Guangdong Academy of Medical Sciences Guangzhou China Xinjuan Fan Department of Pathology The Sixth Affiliated Hospital of Sun Yat-Sen University 26 Erheng Road Guangzhou 510655 China. Yanfen Cui Department of Radiology Shanxi Cancer Hospital Shanxi Medical University No. 3 Xinjie West Alley Taiyuan 030013 China. Zaiyi Liu Department of Radiology Guangdong Provincial People’s Hospital (Guangdong Academy of Medical Sciences) Southern Medical University 106 Zhongshan Er Road Guangzhou 510080 China. Contribution: Formal analysis (equal) Methodology (equal) Writing - original draft (equal) Writing - review & editing (equal) Ke Zhao Depa

Background With the advance in digital pathology and artificial intelligence (AI)-powered approaches, necrosis is proposed as a marker of poor prognosis in colorectal cancer (CRC). However, most previous studies quantified necrosis merely as a tissue type and patch-level segmentation. Thus, it was worth exploring and validating the prognostic and predictive value of necrosis proportion with a pixel-level segmentation in large multicenter cohorts. Methods A semantic segmentation model was trained with 12 tissue types labeled by pathologists. Segmentation was performed using the U-net model with a subsequently derived necrosis tumor ratio (NTR). We proposed the NTR score (NTR-low or NTR-high) to evaluate the prognostic and predictive value of necrosis for disease-free survival (DFS) and overall survival (OS) in the development ( N = 443) and validation cohorts ( N = 333) using 75% as a threshold. Results The 2-category NTR was an independent prognostic factor and NTR-low was associated with significant prolonged DFS (unadjusted HR for high vs. low 1.72 [95% CI 1.19–2.49] and 1.98 [1.22–3.23] in the development and validation cohorts). Similar trends were observed for OS. The prognostic value of NTR was maintained in the multivariate analysis for both cohorts. Furthermore, a stratified analysis showed that NTR-high was a high risk with adjuvant chemotherapy for OS in stage II CRC ( p = 0.047). Conclusion AI-based pixel-level quantified NTR has a stable prognostic value in CRC associated with unfavorable survival. Additionally, adjuvant chemotherapy provided survival benefits for patients with a high NTR score in stage II CRC.

关键词： artificial intelligence colorectal cancer digital pathology necrosis whole-slide images

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Cover Image, Volume 6, Issue 2

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Health Science Reports 2023年第2期6卷

作者： Emmanouil Giorgakis Tommy Ivanics David Wallace Allison Wells Julius Balogh Hailey Hardgrave Derek Krinock Garrett Klutts Lyle Burdine Andrew Singer Amit Mathur Division of Transplant Surgery University of Arkansas for Medical Sciences Little Rock Arkansas USA Contribution: Conceptualization Funding acquisition Investigation Methodology Project administration Resources Supervision Validation Visualization Writing - original draft Writing - review & editing Multi-Organ Transplant Department Universit Health Network Toronto Canada Contribution: Methodology Writing - review & editing Institute of Liver Studies King's College Hospital London UK Contribution: Writing - review & editing Contribution: Data curation Formal analysis Methodology Software Department of Anesthesiology University of Arkansas for Medical Sciences Little Rock Arkansas USA Department of Surgery University of Arkansas for Medical Sciences Little Rock Arkansas USA Contribution: Funding acquisition Resources Writing - review & editing Division of Transplant Surgery Mayo Clinic Phoenix Arizona USA

The cover image is based on the Research LetterAcuity circles allocation policy impact on waitlist mortality and donation after circulatory death liver transplantation: A nationwide retrospective analysisby Emmanouil ...

The cover image is based on the Research Letter Acuity circles allocation policy impact on waitlist mortality and donation after circulatory death liver transplantation: A nationwide retrospective analysis by Emmanouil Giorgakis et al., https://***/10.1002/hsr2.1066

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A Universal Molten Salt Method for Direct Upcycling of Spent Ni-rich Cathode towards Single-crystalline Li-rich Cathode

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Angewandte Chemie 2023年第25期135卷

作者： Zuoyu Qin Dr. Ying Zhang Wuqing Luo Tao Zhang Tao Wang Lianshan Ni Haoji Wang Prof. Ning Zhang Prof. Xiaohe Liu Jiang Zhou Prof. Gen Chen School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials Central South University 410083 Changsha Hunan P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Writing - original draft (lead) Zhongyuan Critical Metals Laboratory and School of Chemical Engineering Zhengzhou University 450001 Zhengzhou Henan P. R. China Contribution: Investigation (supporting) Visualization (lead) Writing - review & editing (equal) Contribution: Validation (lead) Contribution: Investigation (supporting) Resources (lead) Visualization (supporting) School of Metallurgy and Environment Central South University 410083 Changsha Hunan P. R. China Contribution: Investigation (supporting) Writing - review & editing (supporting) College of Chemistry and Chemical Engineering Central South University 410083 Changsha Hunan P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Validation (supporting) Writing - review & editing (supporting) Contribution: Methodology (supporting) Writing - review & editing (supporting) Contribution: Project administration (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (lead) Project administration (supporting) Supervision (supporting) Writing - review & editing (lead) Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (equal) Project administration (lead) Supervision (lead)

With ever-increasing pursuit for high-value output in recycling spent lithium-ion batteries (LIBs), traditional recycling methods of cathodes tend to be obsolete because of the complicated procedures. Herein, we first upcycle spent polycrystal LiNi 0.88 Co 0.095 Al 0.025 O 2 (S-NCA) to high value-added single-crystalline and Li-rich cathode materials through a simple but feasible LiOH-Na 2 SO 4 eutectic molten salt strategy. The in situ X-ray diffraction technique and a series of paratactic experiments record the evolution process of upcycling and prove that excessive Li occupies the transition metal (TM) layers. Beneficial from the single-crystalline and Li-rich nature, the regenerated NCA (R-NCA) exhibits remarkably enhanced electrochemical performances in terms of long-term cyclability, high-rate performance and low polarization. This approach can also be successfully extended to other cathode materials e.g., LiNi x Co y Mn z O 2 (NCM) and mixed spent NCAs with varied degree of Li loss.

关键词： Li-Rich Cathode Single-Crystalline Spent LiNi0.88Co0.095Al0.025O2 Upcycling

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A Highly Twisted Carbazole-Fused DABNA Derivative as an Orange-Red TADF Emitter for OLEDs with Nearly 40 % EQE

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Angewandte Chemie 2022年第47期134卷

作者： Ying-Chun Cheng Xiao-Chun Fan Feng Huang Xin Xiong Jia Yu Dr. Kai Wang Prof. Chun-Sing Lee Prof. Xiao-Hong Zhang Institute of Functional Nano & Soft Materials (FUNSOM) Joint International Research Laboratory of Carbon-Based Functional Materials and Devices Soochow University Suzhou Jiangsu 215123 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Methodology (supporting) Contribution: Data curation (supporting) Contribution: Formal analysis (supporting) Contribution: Project administration (supporting) Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou Jiangsu 215123 P. R. China Contribution: Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead) Center of Super-Diamond and Advanced Films (COSDAF) and Department of Chemistry City University of Hong Kong Hong Kong SAR P.R. China Contribution: Project administration (lead) Supervision (lead) Validation (lead) Contribution: Project administration (lead) Resources (lead) Supervision (lead)

Multiple resonance (MR) type thermally activated delayed fluorescence (TADF) material is currently a research hotspot in organic light-emitting diodes (OLEDs) due to their high color purity and high exciton utilization. However, there are only a handful of MR-TADF emitters with emissions beyond the blue-to-green region. The very limited emission colors for MR-TADF emitters are mainly caused by the fact that so far molecular modifications of MR-TADF do not offer much change in the emission colors. Here, we report a new approach to modifying a prototypical MR core of DABNA by fusing carbazoles to the MR framework. The carbazole-fused molecule (TCZ-F-DABNA) basically maintains the MR-dominated features of DABNA while red-shifting the emission. Its OLED achieves an external quantum efficiency of 39.2 % with a peak at 588 nm, which is a record-high efficiency for OLEDs with peaks beyond 560 nm. This work provides a new approach for significantly tunning emission colors of MR-TADF emitters.

关键词： Carbazole Fusion Concentration Quenching Multiple Resonance Organic Light-Emitting Diodes Thermally Activated Delayed Fluorescence

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In Situ Polymerized 1,3-Dioxolane Electrolyte for Integrated Solid-State Lithium Batteries

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Angewandte Chemie 2023年第12期135卷

作者： Ye Qian Mi Wei Deng Chaohui He Prof. Dr. Osman Eksik Yi Ping Zheng De Kun Yao Dr. Xian Bin Liu Yan Hong Yin Ye Sheng Li Prof. Dr. Bao Yu Xia Prof. Dr. Zi Ping Wu Ganzhou Key Laboratory of Advanced Metals and Functional Materials Faculty of Materials Metallurgy and Chemistry Jiangxi University of Science and Technology Ganzhou 341000 China Contribution: Data curation (lead) Contribution: Formal analysis (lead) Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Wuhan National Laboratory for Optoelectronics School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China Institute of Nanotechnology Gebze Technical University Gebze 41400 Turkey Contribution: Investigation (equal) Contribution: Methodology (lead) Contribution: Supervision (equal) Writing - original draft (lead) Contribution: Resources (lead) Contribution: Conceptualization (lead) Supervision (lead) Visualization (lead) Writing - review & editing (equal) Contribution: Project administration (lead) Supervision (lead) Validation (lead) Writing - original draft (lead)

Solid-state lithium batteries are promising and safe energy storage devices for mobile electronics and electric vehicles. In this work, we report a facile in situ polymerization of 1,3-dioxolane electrolytes to fabricate integrated solid-state lithium batteries. The in situ polymerization and formation of solid-state dioxolane electrolytes on interconnected carbon nanotubes (CNTs) and active materials is the key to realizing a high-performance battery with excellent interfacial contact among CNTs, active materials and electrolytes. Therefore, the electrodes could be tightly integrated into batteries through the CNTs and electrolyte. Electrons/ions enable full access to active materials in the whole electrode. Electrodes with a low resistance of 4.5 Ω □ −1 and high lithium-ion diffusion efficiency of 2.5×10 −11 cm 2 s −1 can significantly improve the electrochemical kinetics. Subsequently, the batteries demonstrated high energy density, amazing charge/discharge rate and long cycle life.

关键词： Interface Lithium Battery Polymerization Solid-State Electrolyte

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Conferring BiVO4Nanorods with Oxygen Vacancies to Realize Enhanced Sonodynamic Cancer Therapy

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Angewandte Chemie 2022年第44期134卷

作者： Dr. Zhuang Yang Dr. Meng Yuan Dr. Bin Liu Dr. Wenying Zhang Dr. Aziz Maleki Prof. Baolin Guo Prof. Ping'an Ma Prof. Ziyong Cheng Prof. Jun Lin State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Changchun 130022 P. R. China School of Applied Chemistry and Engineering University of Science and Technology of China Hefei 230026 P. R. China Contribution: Investigation (lead) Methodology (lead) Resources (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Conceptualization (equal) Investigation (equal) Software (lead) Contribution: Formal analysis (supporting) Funding acquisition (supporting) Methodology (supporting) Contribution: Data curation (supporting) Project administration (supporting) Resources (supporting) Zanjan Pharmaceutical Nanotechnology Research Center (ZPNRC) and Department of Pharmaceutical Nanotechnology School of Pharmacy Zanjan University of Medical Sciences Zanjan 45139-56184 Iran Contribution: Methodology (supporting) Resources (supporting) State Key Laboratory for Mechanical Behavior of Materials and Frontier Institute of Science and Technology and Key Laboratory of Shaanxi Province for Craniofacial Precision Medicine Research College of Stomatology Xi'an Jiaotong University Xi'an 710049 P. R. China Contribution: Investigation (supporting) Validation (supporting) Contribution: Formal analysis (supporting) Software (supporting) Visualization (supporting) Guangdong Provincial Key Laboratory of Research and Development of Natural Drugs School of Pharmacy Guangdong Medical University Guangdong Medical University Key Laboratory of Research and Development of New Medical Materials Dongguan 523808 P. R. China Contribution: Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Resources (lead) Visualization (lead) Writing - review & editing (lead)

Owing to the high depth of tissue penetration, non-invasiveness, and controllability, ultrasound (US)-mediated sonodynamic therapy (SDT) has shown broad application prospects for tumor treatment. However, the electron-hole separation inefficiency of sonosensitizers and the tumor hypoxia remain two major challenges limiting the effect of SDT. Here, ultrafine photoetched bismuth vanadate (BiVO 4 ) nanorods modified with DSPE-PEG 2000 (PEBVO@PEG NRs) were fabricated to achieve in situ self-supply of oxygen (O 2 ) and reactive oxygen species (ROS) for hypoxic tumor therapy. The photoetching approach could enhance the charge separation by inducing enriched oxygen vacancies on the surface of BiVO 4 , thereby improving the generation efficiency of ROS and O 2 . The PEBVO@PEG overcome the main obstacles of traditional sonosensitizers in the SDT process and show promising sonodynamic therapeutic effects, thus providing new strategies for improving the performance of sonosensitizer and hypoxic tumor elimination.

关键词： Bismuth Vanadate Sonodynamic Therapy Sonosensitizers Surface Oxygen Vacancies Ultrasound

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