Browse Articles

Outside Back Cover: Engineering a Meltable MOF to Tune Liquid Transition and Promote Coenzyme Regeneration (Angew. Chem. Int. Ed. 32/2025)

The TouCAN Codebook: Detecting textual misunderstanding in doctor-patient communication with the philosophy of language tools

Effective communication is widely recognized as a cornerstone of successful medical treatment, as extensively documented in prior research. The doctor-patient relationship relies on clear, accurate information exchange to ensure precise diagnoses, treatment adherence, and patient satisfaction. Yet misunderstandings can seriously undermine this process, creating barriers to optimal care and weakening the therapeutic alliance—a critical element of effective healthcare. Consequently, identifying, understanding, and addressing these misunderstandings is essential. This paper introduces a novel approach to detecting and analyzing such misunderstandings in clinical interactions by drawing on concepts from the philosophy of language. Specifically, we present the ToUCAN Codebook, a structured framework designed to systematically classify and examine instances of textual miscommunication in doctor-patient dialogues. By offering a clear methodology for identifying and preventing potential communication breakdowns, the ToUCAN Codebook contributes to improved healthcare outcomes and a deeper understanding of the dynamics that shape medical discourse.

Electrophotochemical Radical Relay for Remote Alkenylation of Unactivated C(sp ³ )–H Sites in Alcohols

Abstract The Mizoroki–Heck reaction is a powerful method for alkene formation from various molecules; however, its application has traditionally been limited to halogenated compounds. Accessing organic molecules with halogen atoms at specific positions in aliphatic systems is highly restricted, and their synthesis is extremely difficult. Therefore, achieving site‐selective alkenylation of alkyl compounds at specific positions remains challenging. This paper presents a versatile redox‐neutral method for the alkenylation of long‐chain alkyl alcohols at unactivated δ‐C(sp 3 )‐H sites, enabling the construction of alkenols through electrophotochemical (EPC) cerium (Ce) catalysis with free alcohols. The method demonstrates excellent substrate compatibility, facilitating the use of both primary and secondary alcohols and enabling the successful synthesis of quaternary carbon alkenols. Mechanistically, cyclic voltammetry experiments reveal that the oxidative reaction is driven by electrochemical oxidation at the anode under applied potential. Additionally, styrene boronic acid remains unoxidized during the reaction, confirming a radical addition mechanism rather than a radical–radical coupling process. UV–vis experiments further demonstrate that the ligand not only activates the alkene boronic acid but also functions as a base to promote the ligand exchange between alcohol and Ce(IV)−Cl species.

The functional connectivity between dorsal-medial prefrontal cortex and middle cingulate cortex links trait rumination and depressive symptoms

Task-based functional neuroimaging has revealed that rumination is associated with functional activations in the default mode network (DMN). The present study aimed to examine whether resting state functional connectivity (FC) within the DMN is associated with individual differences in trait rumination. Using the seed-based functional connectivity analysis in a relatively large sample of late adolescents, this study investigated the neural correlates of trait rumination and their associations with depressive symptoms. Results showed that higher functional connectivity between the left dorsal medial prefrontal cortex (DMPFC) and middle cingulate cortex (MCC) was positively associated with trait rumination. Additionally, stronger FC between the left DMPFC and the right inferior parietal lobe (IPL) was also related to trait rumination. Furthermore, logistic regression analysis indicated that FC strength between the left DMPFC and MCC was significantly associated with depressive symptom severity. These findings suggest DMPFC-related network may reflect neural mechanisms linked to both trait rumination and depressive symptoms in late adolescence.

Mental health and gestational weight gain: A comparison between Brazilian cohorts

Introduction The mental health of pregnant women is critical as it influences both maternal and neonatal outcomes. This study investigates the association between maternal mental health and gestational weight gain (GWG) in two Brazilian cohorts conducted in different periods. Methods The Jundiaí cohort (1997–2000) included 875 pregnant women, while the Araraquara cohort (2017–2024) evaluated mental health of 556 pregnant women from 2017 to 2019. Maternal mental health was assessed using the General Health Questionnaire (GHQ), the State-Trait Anxiety Inventory (STAI), and the Perceived Stress Scale (PSS) during the first, second, and third trimesters. GWG was categorized as adequate, insufficient, or excessive based on Institute of Medicine guidelines. Statistical analysis included bivariate tests (Kruskal-Wallis, chi-square, or Fisher’s exact test) and multinomial ordinal logistic regression to evaluate associations. Results In the Jundiaí cohort, high stress levels in the first trimester were associated with lower odds of insufficient GWG (adjusted OR for second quartile: 0.36, 95% CI: 0.18–0.71). In the second trimester, high anxiety levels (TAI ≥ 40) were associated with higher odds of insufficient GWG (ORa: 1.76, 95% CI: 1.12–2.76). In the third trimester, high stress levels (PSS fourth quartile) were associated with higher odds of insufficient GWG (adjusted OR: 1.72, 95% CI: 1.02–2.91). In the Araraquara cohort, no significant associations between mental health and GWG were found. Conclusions Our findings highlight the importance of incorporating psychosocial support in prenatal care to improve maternal and neonatal outcomes. Variations in socioeconomic and temporal contexts may influence the relationship between mental health and GWG. Future research should explore the underlying mechanisms and develop interventions tailored to different socioeconomic and temporal contexts.

Cooperative Ammonia Formation Catalyzed by Molybdenum and Samarium Complexes

Abstract A series of novel samarium complexes bearing cyclopentadienyl–amide chelate ligands were synthesized and characterized by X‐ray analysis. The complexes function as effective proton‐coupled electron transfer (PCET) catalysts, facilitating molybdenum‐catalyzed ammonia formation from dinitrogen under ambient conditions. In this reaction system, the Sm complexes could be recycled over 300 times, and they increased the ammonia formation rate by sevenfold compared to that obtained for reactions occurring in the absence of such complexes. Experimental results and density functional theory calculations indicate that the Sm complexes undergo protonation and reduction to form Sm(II) complexes, which then accelerate proton and electron transfer to the Mo complexes via PCET processes from the terminal proton source and reductant. This paper presents the first successful example of Sm complexes that can function as efficient catalysts for 300 cycles, promoting proton and electron transfer in Mo‐catalyzed ammonia formation.

Computing mutual similarity of 3D human faces in nearly linear time

Using three-dimensional scans of human faces has become an emerging technique in studies of human variation, where the quantitative assessment of facial similarity complements the measurement of other somatic traits. While the algorithms for automated registration (geometrical alignment) and similarity measurement of two facial scans are well-known and used in practice, their direct application for batch processing is limited due to computational requirements. The batch N:N analysis, where all pairs of scans in a dataset must be mutually registered and compared, introduces quadratic complexity with computation times reaching hours even for relatively small datasets, making it practically unusable. This paper presents a rapid and accurate approach with nearly linear time complexity. Our solution utilizes properties of facial scan geometry to optimize individual steps. Moreover, the algorithm deals with possible holes and other artifacts in polygonal meshes automatically. Experiments demonstrate that the proposed solution is very fast and sufficiently accurate compared to a precise quadratic-time baseline approach.

Interfacial‐Confined Oxygen Vacancy Clusters in ZrO ₂ ‐Supported In ₂ O _3‐ <i> _x </i> Catalysts Boost Methanol Production From CO ₂

Abstract Oxygen vacancies (V O ) play a vital role in catalytic reactions. Tuning the V O structures beyond its density is of great significance for optimizing catalytic performance, but remains challenging due to uncontrolled reduction and its poor stability under reaction conditions. Here, we report that the integration of quantum size effect for enhanced In 2 O 3 reducibility with strong In–O–Zr interfacial confinement for high stability enables the creation of stable large‐size V O clusters (e.g., trimers, tetramers, and larger) on ZrO 2 ‐supported monolayer In 2 O 3‐ x nano‐islands with high density without overreduction to metallic indium. In the CO 2 hydrogenation reaction, the ZrO 2 ‐supported monolayer In 2 O 3‐ x catalyst with V O clusters exhibits a considerably higher intrinsic activity for methanol production than that of bulk In 2 O 3 with single V O sites. Further addition of Pd onto these monolayer In 2 O 3‐ x with enriched V O clusters allows achieving an unprecedentedly high methanol space‐time yield of 46.6 mmol MeOH ·g cat −1  h −1 at 270 °C along with long‐term stability for at least 200 h, surpassing all In 2 O 3 ‐based catalysts reported to date.

The evolution of comorbidities in chronic diseases among Chinese middle-aged and elderly people: Evidence from the CHARLS (2015-2020)

Background The comorbidity of chronic diseases among middle-aged and elderly people is a global public health concern that has attracted great attention in recent years. It is crucial to explore the evolutionary pattern of chronic disease comorbidity in Chinese middle-aged and elderly people and to reveal the developmental trajectory of chronic diseases in this population. Methods Data from the China Health and Retirement Longitudinal Study (CHARLS 2015–2020) were utilized for the fixed cohort analysis. Based on the prevalence information of 14 chronic diseases (including hypertension, dyslipidemia, diabetes, cancer, chronic lung diseases, liver disease, heart disease, stroke, kidney disease, stomach diseases, emotional problems, memory-related diseases, arthritis, and asthma) among 10,089 participants aged ≥45 years, association rules and cluster analysis were used to identify trends and trajectories of comorbidities in the middle-aged and elderly populations in China. Results The analysis revealed that the comorbidity rate of the 14 chronic diseases showed a consistent annual increase from 2015–2020. By 2020, over 85% of patients diagnosed with a single chronic condition exhibited concurrent multimorbidity. This epidemiological progression was paralleled by a progressive increase in detected disease associations: binary comorbidities rose from three significant associations in 2015–10 in 2020, whereas higher-order combinations expanded from one ternary association in 2015–35 ternary and 18 quaternary associations by 2020. Notably, hypertension maintained a central position across all identified comorbidity clusters. The comorbidity patterns identified in 2015 included respiratory, liver and kidney, and cardio-cerebral comorbidity patterns and cancer and emotional problems. The comorbidity patterns identified in 2018 included respiratory, liver and kidney, cerebrovascular, and cardiovascular metabolic comorbidity patterns. The comorbidity pattern in 2020 was the same as that in 2018. Conclusion The issues of comorbidities in chronic diseases among Chinese middle-aged and elderly people is significant, with observed variations in the comorbidity patterns across different time periods. The development of clinical assessment and management guidelines for chronic diseases comorbid with key conditions, such as hypertension and dyslipidemia, is recommended. These guidelines aim to facilitate the co-management, co-treatment, and co-reduction of multiple diseases among middle-aged and elderly people.

Expression of concern: Water, sanitation, and hygiene conditions and prevalence of intestinal parasitosis among primary school children in Dessie City, Ethiopia

Healthcare utilization associated with antimicrobial resistance at a tertiary hospital in Vietnam: A retrospective observational study from 2016 to 2021

Background Despite the increasing burden of antimicrobial resistance (AMR), specifically on priority ESKAPE pathogens, studies examining the economic impact of AMR in low- and lower-middle-income countries have been scarce and require further investigation to optimize the post-COVID resource allocation. Objectives To quantify the incremental hospital costs and length of stay (LOS) associated with antimicrobial-resistant versus -susceptible among priority ESKAPE pathogens from the healthcare sector perspective. Methods We conducted a retrospective observational study of patients hospitalized at the Hospital for Tropical Diseases from 2016−2021 with non-duplicate isolates of any ESKAPE pathogens from clinical specimens. The patients were then stratified into resistant- and susceptible- groups by the WHO classification. Multivariate generalized linear regression and negative binomial regression with linear spline at COVID-19 occurrence were employed to evaluate the incremental hospital costs and LOS due to AMR, respectively. These regressions were adjusted for sociodemographic and clinical characteristics. We applied difference-in-difference (DiD) to estimate the differential cost between resistant and susceptible groups regarding COVID-19 change. Results During the six-year period, 4,197 out of 6,670 patients (62.92%) were isolated with priority pathogens, with the highest prevalence of priority pathogens observed in 3GCREC and MRSA (accounting for 45.63% and 25.33%, respectively). After covariate adjustments, the incremental hospital costs per resistant patient were significantly higher across most pathogens except for patients tested with MRSA results (average CRAB $3,980; CRPA $1,000; 3GCREC $444; 3GCRKP $1,942; MRSA -$326), while incremental LOS ranged from 1.40 days for 3GCREC (95%CI: 0.69–2.10 ) to 12.54 days for CRPA (95%CI: 11.12–13.97). COVID-19 significantly enlarged the hospital cost gaps between patients with antibiotic-resistant and antibiotic-susceptible profiles, with A.baumannii (CRAB vs. CSAB) showing the highest DiD at $9,116 (95%CI: $6,019-$12,213). Conclusion The incremental hospital costs of AMR were significant, with the highest one observed in CRAB patients, and the difference between resistant and susceptible cases widened during the COVID-19 pandemic.

Correction: Impact of prolonged social crisis on resilience and coping indicators

Scalable H ₂ O ₂ Production via O ₂ Reduction Using Immobilized Vanadyl Phthalocyanine

Abstract The production of hydrogen peroxide (H 2 O 2 ) via the two‐electron oxygen reduction reaction (ORR) has emerged as a promising alternative to the conventional anthraquinone process. However, achieving selective H 2 O 2 production at practically relevant current densities (i.e., ampere‐level) remains challenging due to significant selectivity deterioration at high rates. In this study, we develop a composite catalyst by immobilizing vanadyl phthalocyanine (VOPc) on carbon nanotube (CNT) substrates and evaluate its performance under conditions relevant to practical ORR electrolysis. Encouragingly, the VOPc/CNT catalyst composite achieves a high ORR current density of up to 3.5 A cm −2 with over 90% selectivity toward H 2 O 2 in acidic media. Through various in situ characterizations and theoretical calculations, we reveal that the structural integrity of the vanadium catalytic center in VOPc plays a pivotal role in stabilizing *OOH adsorption and impeding O─O cleavage under high cathodic potentials, which is critical for achieving high H₂O₂ selectivity at elevated current densities.

“Rigid Exterior, Soft Interior” Design Enables High‐Voltage Polyether Electrolytes for Quasi‐Solid‐State Batteries

Abstract Polyether electrolytes with high Li + conductivity and excellent interfacial contact have garnered significant attention. Yet further applications of such electrolytes in high‐voltage lithium metal batteries are severely hindered by the instability of the electrolyte and electrolyte/electrodes interphases. Here, we report a novel high‐voltage polyether electrolyte with a “rigid exterior, soft interior” design, which involves a 3D F‐contained network as a rigid exterior framework, and a unique solvation structure with intensified Li + ‐anion coordination as a soft interior within the framework. The achieved electrolyte demonstrates an ionic conductivity of 1.13 mS cm −1 at 25 °C, a Li + transference number of 0.85, and an extended electrochemical stability window of over 5 V. Besides, such a designed polyether electrolyte further induces salt‐philic, solvent‐phobic interfacial films for stabilizing electrolyte/electrode interphases. An exceptional cyclability in a Li||Li cell for over 4000 h, and a preferable capacity and cyclability in even 4.6 V Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) quasi‐solid‐state batteries (QSSBs) are demonstrated. Meanwhile, the resulting 4.3 V Li||LiNi 0.5 Co 0.2 Mn 0.3 O 2 QSSB shows a Coulombic efficiency of ∼100% and an extremely high capacity retention of 95.4% after 600 cycles at 3C. A capacity retention of over 96.3% after 400 cycles at 1C are further realized in 4.5 V Li||NCM811 QSSB.

Catalytic α‐Site‐Selective Hydrogen‐Deuterium Exchange of Benzylic Alcohols by Palladium Single‐Atom Catalyst

Abstract Catalytic hydrogen‐deuterium exchange (HDE) has emerged as a valuable tool for achieving site‐selective deuteration and the precision labeling of bioactive molecules. Incorporation of deuterium at metabolically labile positions, enabled by such methods, can potentially improve drug efficacy through the kinetic isotope effect. However, achieving precise, site‐selective incorporation of deuterium at specific molecular positions remains challenging. Herein, we report a highly efficient α‐site‐selective HDE of benzylic alcohols via a palladium single‐atom catalyst (Pd SAC). By using the Pd SAC, exceptional activity and selectivity in HDE reactions were achieved, delivering up to 95% deuterium incorporation (D‐inc.) at the α‐position while effectively suppressing undesired pathways (e.g., α,β‐multisite deuteration). Mechanistic investigations reveal that the Pd SAC promotes site‐selective HDE through two distinct surface pathways: (i) a previously unreported direct C─H bond activation and (ii) a modified borrowing hydrogen process in which high‐pressure hydrogen inhibits the keto enol tautomerization, thereby largely circumvents α,β‐multisite deuteration. The catalyst exhibits robust stability, reusability, and broad substrate compatibility, underscoring its potential for practical applications. This work marks a significant advance in heterogeneous single‐atom catalytic methodologies for site‐selective deuteration, offering a complementary solution to longstanding challenges in catalytic organic synthesis.

A Platform for the Development of Highly Red‐Shifted Azobenzene‐Based Optical Tools

Abstract Azobenzenes are versatile photoswitches that can be used to generate elaborate optical tools, including photopharmaceuticals. However, the targeted application‐guided design of new photoswitches with specific properties remains challenging. We have developed synthetic protocols for derivatives of the dfdc (di‐ ortho‐ fluoro‐di‐ ortho‐ chloro) azobenzene scaffold with chemical alterations in the para ‐/ ortho ‐positions and performed an in‐depth study into the effects of their structures on their photophysical properties with an emphasis on the n → π* absorption band using NMR, UV–vis, and X‐ray analysis. The data was used to establish and validate a computational approach that allows to compute realistic UV–vis spectra by combining TD‐DFT excited‐state calculations from 6000 thermally accessible structures generated through MD simulations while considering the high structural flexibility of ortho ‐substituted azobenzenes. We added 15 new visible light‐operated photoswitches to the toolbox for the development of optical devices with relaxation rates across multiple orders of magnitude and identified several examples with stronger bathochromic shifts than the dfdc azobenzene lead structure. Our combined experimental and computational study forms the foundation for the advanced in silico design and synthesis of new highly red‐shifted photoswitches. To showcase the potential of dfdc azobenzenes for the development of chemical tools, we synthesized dfdc ‐OptoBI‐1 and demonstrated its biological activity as a red light‐operated activator of TRPC6 channels in HEK293 cells.

Selective Production of Acetylene from the C─C Coupling Reaction of CH ₄ with CO ₂ Mediated by Ta ₂ O ₂ ⁺ Cluster Cations

Abstract Coconversion of methane and carbon dioxide to C 2 hydrocarbons via the C CH4 ─C CO2 coupling reaction is of great significance to mitigate greenhouse effect and develop an alternative route for manufacture of important industrial feedstocks (e.g., C 2 H 2 ), however, it has not yet been achieved so far owing to the difficulty in breaking both of the C═O bonds in CO 2 as well as the precise control of sequential elementary reactions targeted for C 2 hydrocarbons. Herein, by using the tantalum oxide Ta 2 O 2 + as an active cluster, an unprecedented C CH4 ─C CO2 coupling reaction of CH 4 with CO 2 to exclusively produce the C 2 hydrocarbon of C 2 H 2 has been successfully realized even at room temperature by the state‐of‐the‐art mass spectrometry. The in situ reconstruction from Ta─O─Ta cluster skeleton to tantalum carbide Ta─C─Ta experienced upon the prereaction with CH 4 is critical to delicately control the sequential elementary reactions targeted for C 2 H 2 generation. This finding not only leads to a breakthrough in the field of gas‐phase and condensed‐phase chemistry wherein the C 2+ oxygenated compounds were the mainstream products for C CH4 ─C CO2 coupling of CH 4 with CO 2 , but also explores a new active structure and a novel reaction mechanism beneficial for selective production of C 2 hydrocarbons from coconversion of CH 4 and CO 2 .

Multivariate MOF Hollow Fiber Membranes with Precision‐Tuned Subnanometer Channels Toward Aromatic Hydrocarbon Separation

Abstract Metal‐organic framework (MOF) membranes exhibit great potential for molecular separations, but it remains a considerable challenge to achieve precise pore aperture regulation, typically requiring the synthesis of distinct MOF structures for each targeted separation. Herein, the first multivariate MOF (MTV‐MOF) hollow fiber membranes with precision‐tuned subnanometer channels have been fabricated by leveraging the heterogeneous spatial distribution of ligands, where reduced coordination energy barriers drive the formation of alternating narrow (local‐path limited) and wide channels, simultaneously addressing the critical permeability‐selectivity trade‐off in membrane separations. The alternating narrow‐wide channel architecture has been systematically investigated through combined density functional theory calculation, molecular dynamics simulation and mathematical modeling, with direct experimental validation provided by low‐dose high‐resolution scanning transmission electron microscopy and quantitative adsorption analysis. These MTV‐MOF membranes demonstrated the ability to selectively separate aromatic hydrocarbons achieving highly selective separation while reduce the molecular transport barriers, offering significant potential for industrial separation processes.

Non‐Innocent Ligands as Mediators for Visible‐Light‐Initiated Element–Carbon Bond Homolysis in Main Group Chemistry

Abstract Photoinitiated homolysis of element–carbon bonds is an important method for the generation of carbon‐centered radicals in catalysis and organometallic or polymer chemistry. In this respect, the use of earth‐abundant main group elements such as aluminum or silicon is attractive. Generally, subvalent species derived from these typically redox‐inactive elements are unstable and within their high‐valent configuration +III (Al) or +IV (Si) comparatively strong E─C bonds are formed. Therefore, E─C homolysis usually requires shortwave UV irradiation, which hampers their use as radical sources. Some reports in the literature show that visible‐light‐induced E─C homolysis is possible when a redox non‐innocent ligand (NIL) is coordinated to the organometallic fragment. In a simplified view, the NILs provide chromophoric moieties, which can absorb energy in form of light and subsequently convert it to break the element–carbon bonds. The resulting main group element radicals are in turn stabilized by delocalization of the unpaired electron, effectively lowering the dissociation energy of the E─C bond. In this article, the effects of NILs as mediators for visible‐light‐induced E─C bond homolysis in main group chemistry are discussed on the basis of selected literature reports, and future opportunities and challenges are highlighted.

Prevalence, associated risk factors and satellite imagery analysis in predicting soil-transmitted helminth infection in Nakhon Si Thammarat Province, Thailand

Abstract Soil-transmitted helminth (STH) infections remain a significant public health concern in rural areas, often leading to nutritional and physical impairment, particularly in children. This study aimed to assess the prevalence and associated factors of STH infections among schoolchildren in Thasala District, Nakhon Si Thammarat Province, Thailand, and to develop a predictive model for identifying high-risk areas using satellite imagery data. A cross-sectional study was conducted with 319 primary schoolchildren from six sub-districts in Thasala District. Stool samples were analyzed for STH infections using the formalin ethyl acetate concentration technique (FECT) and agar plate culture (APC), while behavioral data were collected through questionnaires to identify key risk factors. We developed an innovative predictive model by integrating convolutional neural networks (CNNs) for land-use classification of satellite imagery with artificial neural networks (ANNs) following dimensionality reduction through principal component analysis (PCA). The STH infections were detected in 31 samples (9.72%), with higher prevalence in males (11.38%) than females (8.67%). Mono-infections predominated, with Trichuris trichiura (5.02%) and hookworm (3.49%) being the most frequent. Mixed infections accounted for 1.25%, primarily co-infections of hookworm with T. trichiura (0.94%) or Strongyloides stercoralis (0.31%). Not cutting nails was identified as a significant behavioral factor associated with STH infections (p = 0.047), while other behavioral factors showed no statistical significance. From the satellite imagery analysis, specific environmental features, particularly higher proportions of agricultural land and closer proximity to water bodies, were positively associated with elevated STH prevalence. The modelling approach generated spatial risk maps for STH infections, providing a cost-effective tool for identifying high-risk transmission zones. These findings highlight that STH infections persist among rural Thai schoolchildren, with poor hygiene practices as a contributing factor. Strengthening hygiene education, improving sanitation, and implementing targeted environmental interventions are essential for effective control.