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1.
BMC Nurs ; 23(1): 642, 2024 Sep 11.
Article in English | MEDLINE | ID: mdl-39256718

ABSTRACT

BACKGROUND: Loneliness was associated with interpersonal sensitivity, but the factors contributing to this relationship in nursing students remain unclear. This study investigated the relationship between loneliness and interpersonal sensitivity among nursing undergraduates, with a specific focus on the mediating roles played by problematic internet use and bedtime procrastination. METHOD: This study was conducted as a cross-sectional survey at a university in China between November and December 2022. Data were collected using a self-administered online questionnaire that included demographic characteristics, the Three-Item Loneliness Scale (T-ILS), the Chinese Version of Short Form of Interpersonal Sensitivity Measure (IPSM-CS), the 6-item short form of the Problematic Internet Use Questionnaire (PIUQ-SF-6), and the Bedtime Procrastination Scale (BPS). Pearson correlation analysis was employed to explore the relationships among loneliness, interpersonal sensitivity, problematic internet use, and bedtime procrastination. Structural equation modeling (SEM) was conducted using AMOS software to examine the mediating role of problematic internet use and bedtime procrastination between loneliness and interpersonal sensitivity. RESULTS: Loneliness was positively related to interpersonal sensitivity among nursing undergraduates (ß = 0.44, P < 0.001). There was a significant chain mediation role of problematic internet use and bedtime procrastination in the relationship between loneliness and interpersonal sensitivity. CONCLUSIONS: The study contributed to deepening the understanding of the relationship between loneliness and interpersonal sensitivity and provided valuable insights into the improvement of interpersonal sensitivity in nursing undergraduates.

2.
Org Lett ; 2024 Sep 03.
Article in English | MEDLINE | ID: mdl-39226141

ABSTRACT

A highly efficient Au(I)-catalyzed cascade reaction between bispropargylic alcohols and pyridine-N-oxides has been realized. The reaction process involved a gold(I)-catalyzed sequential oxidation/Pinacol rearrangement/oxacyclization. Moreover, 1,2-aryl, 1,2-alkyl, or 1,2-vinyl migration was favored over 1,2-alkynyl in the crucial gold(I)-catalyzed Pinacol rearrangement step. A range of 2,4,5-trisubstituted 3(2H)-furanones were synthesized in high yields (up to 88%) with excellent regioselectivities (up to >19:1) under mild reaction conditions.

3.
Angew Chem Int Ed Engl ; : e202413033, 2024 Sep 04.
Article in English | MEDLINE | ID: mdl-39229697

ABSTRACT

Electrocatalytic nitrate reduction reaction (NO3RR) is a process that requires the participation of eight electrons and nine protons. The regulation of active hydrogen (H*) supply and a deep understanding of related processes are necessary for improving the ammonia yield rate and Faradaic efficiency (FE). Herein, we synthesized a series of atomically precise copper-halide clusters Cu2X2(BINAP)2 (X = Cl, Br, I), among which the Cu2Cl2(BINAP)2 cluster shows the optimal ammonia FE of 94.0% and an ammonia yield rate of 373 µmol h-1 cm-2. In situ experiments and theoretical calculations reveal that halogen atoms, especially Cl in Cu2Cl2(BIANP)2, can significantly affect the distance of alkali metal-ionized water on the catalyst surface, which can promote the water dissociation to enhance the localized H* enrichment for the continues hydrogenation of nitrate to ammonia. This work explains the role of H* in the hydrogenation process of NO3RR and the importance of localized H* enrichment strategy for improving the FEs.

4.
BMC Palliat Care ; 23(1): 201, 2024 Aug 06.
Article in English | MEDLINE | ID: mdl-39107758

ABSTRACT

BACKGROUND: Advance care planning (ACP) can contribute to individuals making decisions about their healthcare preferences in advance of serious illness. Up to now, the acceptance level and associated factors of ACP among the public in China remain unclear. This study aims to investigate the acceptance level of ACP in China and identify factors associated with it based on the socioecological model. METHODS: A total of 19,738 participants were included in this survey. We employed a random forest regression analysis to select factors derived from the socioecological model. Multivariate generalized linear model analysis was then conducted to explore the factors that were associated with the acceptance level of ACP. RESULTS: On a scale ranging from 0 to 100, the median score for acceptance level of ACP was 64.00 (IQR: 48.00-83.00) points. The results of the multivariate generalized linear model analysis revealed that participants who scored higher on measures of openness and neuroticism personality traits, as well as those who had greater perceptions of social support, higher levels of health literacy, better neighborly relationships, family health, and family social status, were more likely to accept ACP. Conversely, participants who reported higher levels of subjective well-being and greater family communication levels demonstrated a lower likelihood of accepting ACP. CONCLUSIONS: This study identified multiple factors associated with the acceptance level of ACP. The findings offer valuable insights that can inform the design and implementation of targeted interventions aimed at facilitating a good death and may have significant implications for the formulation of end-of-life care policies and practices in other countries facing similar challenges.


Subject(s)
Advance Care Planning , Humans , Advance Care Planning/statistics & numerical data , Advance Care Planning/standards , Advance Care Planning/trends , Male , Female , Middle Aged , Adult , China , Surveys and Questionnaires , Aged , Patient Acceptance of Health Care/psychology , Patient Acceptance of Health Care/statistics & numerical data , Adolescent
5.
Angew Chem Int Ed Engl ; : e202410416, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39134476

ABSTRACT

Precise control over the organic composition is crucial for tailoring the distinctive structures and properties of hybrid metal halides. However, this approach is seldom utilized to develop materials that exhibit stimuli-responsive circularly polarized luminescence (CPL). Herein, we present the synthesis and characterization of enantiomeric hybrid zinc bromides: biprotonated ((R/S)-C12H16N2)ZnBr4 ((R/S-LH2)ZnBr4) and monoprotonated ((R/S)-C12H15N2)2ZnBr4 ((R/S-LH1)2ZnBr4), derived from the chiral organic amine (R/S)-2,3,4,9-Tetrahydro-1H-carbazol-3-amine ((R/S)-C12H14N2). These compounds showcase luminescent properties; the zero-dimensional biprotonated form emits green light at 505 nm, while the monoprotonated form, with a pseudo-layered structure, displays red luminescence at 599 and 649 nm. Remarkably, the reversible local protonation-deprotonation behavior of the organic cations allows for exposure to polar solvents and heating to induce reversible structural and luminescent transformations between the two forms. Theoretical calculations reveal that the lower energy barrier associated with the deprotonation process within the pyrrole ring is responsible for the local protonation-deprotonation behavior observed. These enantiomorphic hybrid zinc bromides also exhibit switchable circular dichroism (CD) and CPL properties. Furthermore, their chloride counterparts were successfully obtained by adjusting the halogen ions. Importantly, the unique stimuli-responsive CPL characteristics position these hybrid zinc halides as promising candidates for applications information storage, anti-counterfeiting, and information encryption.

6.
Nurse Educ Today ; 142: 106346, 2024 Aug 11.
Article in English | MEDLINE | ID: mdl-39146919

ABSTRACT

BACKGROUND: Mental health-related stigma remains a complex and pervasive issue globally. It not only inhibits individuals from seeking help but also influences the quality of healthcare they receive. Despite extensive research on mental health-related stigma, there is still limited understanding of factors influencing mental health-related stigma among nursing students. OBJECTIVES: This study aimed to assess the level of mental health-related stigma among Chinese nursing students and investigate possible associated factors. METHODS: Data were collected from the 2023 Psychology and Behavior Investigation of Chinese Residents (PBICR) survey. A total of 967 nursing students were included in the study. Multivariate stepwise linear regression analysis was conducted to examine the influencing factors of mental health stigma. RESULTS: The mean mental health-related stigma score among nursing students was 15.31 ± 5.23 (range = 0-27). Perceived stress (ß = 0.14, P = 0.001), self-efficacy (ß = 0.22, P < 0.001), academic stage (ß = 0.17, P < 0.001), depression (ß = 0.15, P < 0.001), and adverse life events (ß = 0.06, P = 0.044) were significantly associated with mental health-related stigma among nursing students (R2 = 0.147, adjusted R2 = 0.143, F = 33.214, P < 0.001). CONCLUSIONS: Nursing students in China exhibit a moderate level of mental health-related stigma, suggesting room for improvement. Perceived stress, self-efficacy, academic stage, depression, and adverse life events emerged as significant influencing factors for mental health-related stigma. These findings provide valuable insights for developing interventions to reduce mental health-related stigma among nursing students, ultimately enhancing their well-being and preparing them for becoming competent healthcare professionals in the future.

7.
Angew Chem Int Ed Engl ; : e202408310, 2024 Aug 29.
Article in English | MEDLINE | ID: mdl-39210521

ABSTRACT

Coinage metal (Au, Ag, Cu) cluster and polyoxometalate (POM) cluster represent two types of subnanometer "artificial atoms" with significant potential in catalysis, sensing, and nanomedicine. While composite clusters combining Ag/Cu clusters with POM have achieved considerable success, the assembly of gold clusters with POM is still lagging. Herein, we first designedly synthesized two cluster structural units: an Au3O cluster stabilized by diverse N-heterocyclic carbene (NHC) ligands and an amine-terminated POM linker. The subsequent reaction involved amine substitution in the POM linker for the central O atom in the Au3O cluster, resulting in the first ternary composite cluster - a POM cluster sandwiched by two Au clusters protected by NHCs. Single-crystal X-ray diffraction and other characteristic methods characterized their atomically precise structures. Furthermore, altering the NHC ligands decreased the number of gold atoms in the sandwich structures, accompanying the different protonated degrees of amine ligand in the terminal end of the POM linker. These composite clusters showed excellent performances in catalytic H2O2 conversion through the synergistic effect between gold clusters and POM clusters. This work opens a new avenue to functional composite metal clusters and would promote their enhanced catalysis applications through intercluster synergistic interactions within composite systems.

8.
Angew Chem Int Ed Engl ; : e202412144, 2024 Aug 21.
Article in English | MEDLINE | ID: mdl-39169221

ABSTRACT

Thiolate-protected Cu clusters with well-defined structures and stable low-coordinated Cu+ species exhibit remarkable potential for the CO2RR and are ideal model catalysts for establishing structure-electrocatalytic property relationships at the atomic level. However, extant Cu clusters employed in the CO2RR predominantly yield 2e- products. Herein, two model Cu4(MMI)4 and Cu8(MMI)4(tBuS)4 clusters (MMI = 2-mercapto-1-methylimidazole) are prepared to investigate the synergistic effect of Cu+ and adjacent S sites on the CO2RR. Cu4(MMI)4 can reduce CO2 to deep-reduced products with a 91.0% Faradaic efficiency (including 53.7% for CH4) while maintaining remarkable stability. Conversely, Cu8(MMI)4(tBuS)4 shows a remarkable preference for C2+ products, achieving a maximum FE of 58.5% with a C2+ current density of 152.1 mA∙cm-2. In situ XAS and ex situ XPS spectra reveal the preservation of Cu+ species in Cu clusters during CO2RR, extensively enhancing the adsorption capacity of *CO intermediates. Moreover, kinetic analysis and theoretical calculations confirm that S sites facilitate H2O dissociation into *H species, which directly participate in the protonation process on adjacent Cu sites for the protonation of *CO to *CHO. This study highlights the important role of Cu-S dual sites in Cu clusters and provides mechanistic insights into the CO2RR pathway at the atomic level.

10.
Geriatr Nurs ; 58: 480-487, 2024.
Article in English | MEDLINE | ID: mdl-38968651

ABSTRACT

BACKGROUND: Evidence on the differences in depressive symptoms among older adults with multiple chronic conditions (MCCs) in urban and rural areas is limited. METHODS: Measures of depressive symptoms (Center for Epidemiologic Studies Depression Scale-10) and demographic factors (age, gender, and urban-rural distribution) were used. RESULTS: A total of 4021 older adults with MCCs were included in this study. Significant differences were observed in both network global strength (Urban: 3.989 vs. Rural: 3.703, S = 0.286, p = 0.003) and network structure (M = 0.139, p = 0.002) between urban and rural residents. CONCLUSIONS: The study highlights the need for region-specific approaches to understanding and addressing depression and holds the potential to enhance understanding of the psychological health status of older adults with MCCs in urban and rural settings.


Subject(s)
Depression , Rural Population , Urban Population , Humans , Male , Female , Rural Population/statistics & numerical data , Urban Population/statistics & numerical data , Aged , Depression/epidemiology , Depression/psychology , Surveys and Questionnaires , Multiple Chronic Conditions/epidemiology , Multiple Chronic Conditions/psychology , Aged, 80 and over
11.
Support Care Cancer ; 32(7): 420, 2024 Jun 08.
Article in English | MEDLINE | ID: mdl-38850487

ABSTRACT

PURPOSE: This study aims to investigate the Readiness for Return-to-Work (RRTW) of patients with head and neck tumours and to analyse the relationships among self-efficacy, disease uncertainty, psychosocial adaptation, and RRTW in head and neck cancer (HNC) patients. METHODS: A cross-sectional study was conducted with 259 HNC patients with a discharge length of ≥1 month at a tertiary hospital in Liaoning Province. The research tools included a self-designed general information questionnaire, the Readiness for Return-to-Work (RRTW) Scale, the General Self-Efficacy Scale (GSES), the Mishel Uncertainty in Illness Scale (MUIS), and the Self-Reporting Psychosocial Adjustment to Illness Scale (PAIS-SR). Descriptive statistical analysis, the rank sum test, Spearman correlation analysis, and ordered multiple and dichotomous logistic regression analyses were used. RESULTS: The overall RRTW among HNC patients was low (41.9%). HNC patients who did not return to work were mainly in the precontemplation stage (38.1%) and contemplation stage (29.9%). HNC patients who returned to work were mainly in the active maintenance stage (64.2%). Children's status (OR = 0.218, 95% CI 0.068-0.703), self-efficacy (OR = 1.213, 95% CI 1.012-1.454), unpredictability (OR = 0.845, 95% CI 0.720-0.990), occupational environment (OR = 0.787, 95% CI 0.625-0.990), and family environment (OR = 0.798, 95% CI 0.643-0.990) influence the RRTW of HNC patients who have not returned to work. Educational level (OR = 62.196, 95% CI 63.307-68.567), children's status (OR = 0.058, 95% CI 1.004-2.547), self-efficacy (OR = 1.544, 95% CI 3.010-8.715), unpredictability (OR = 0.445, 95% CI 1.271-2.280), and psychological status (OR = 0.340, 95% CI 1.141-2.401) influence the RRTW of HNC patients who have returned to work. CONCLUSION: Children's status, education level, self-efficacy, illness uncertainty, and psychosocial adjustment are crucial to RRTW. This study provides a theoretical basis for formulating intervention measures aimed at improving the RRTW of patients.


Subject(s)
Adaptation, Psychological , Head and Neck Neoplasms , Return to Work , Self Efficacy , Humans , Cross-Sectional Studies , Male , Female , Return to Work/statistics & numerical data , Return to Work/psychology , Head and Neck Neoplasms/psychology , Head and Neck Neoplasms/rehabilitation , Middle Aged , Adult , Surveys and Questionnaires , Aged , China , Uncertainty
12.
Natl Sci Rev ; 11(7): nwae174, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38887544

ABSTRACT

Chemically modified superatoms have emerged as promising candidates in the new periodic table, in which Au13 and its doped M n Au13- n have been widely studied. However, their important counterpart, Ag13 artificial element, has not yet been synthesized. In this work, we report the synthesis of Ag13 nanoclusters using strong chelating ability and rigid ligands, that fills the gaps in the icosahedral superatomic metal clusters. After further doping Ag13 template with different degrees of Au atoms, we gained insight into the evolution of their optical properties. Theoretical calculations show that the kernel metal doping can modulate the transition of the excited-state electronic structure, and the electron transfer process changes from local excitation (LE) to charge transfer (CT) to LE. This study not only enriches the families of artificial superatoms, but also contributes to the understanding of the electronic states of superatomic clusters.

13.
Chem Commun (Camb) ; 60(57): 7374-7377, 2024 Jul 11.
Article in English | MEDLINE | ID: mdl-38922126

ABSTRACT

Detailed photophysical processes of two AuCu14 clusters with different substituents (-F or -C(CH3)3) of the thiol ligand were studied in this work. The electronic effect of the substituents led to structural shrinkage, thus enhancing the luminous intensity. The internal conversion (IC) and intersystem crossing (ISC) rates in the AuCu14-C(CH3)3 crystal were slower compared with the AuCu14-F crystal, which was caused by the steric effect.

14.
J Am Chem Soc ; 2024 Jun 05.
Article in English | MEDLINE | ID: mdl-38838264

ABSTRACT

Chiral atomically precise metal clusters, known for their remarkable chiroptical properties, hold great potential for applications in chirality recognition. However, advancements in this field have been constrained by the limited exploration of host-guest chemistry, involving metal clusters. This study reports the synthesis of a chiral Cu16(C2B10H10S2)8 (denoted as Cu16@CB8, where C2B10H12S2H2 = 9,12-(HS)2-1,2-closo-carborane) cluster by an achiral carboranylthiolate ligand. The chiral R-/S-Cu16@CB8 cluster features chiral cavities reminiscent of cyclodextrins, which are surrounded by carborane clusters, yet they crystallize in a racemate. These cyclodextrin-like cavities demonstrated the specific recognition of amino acids, as indicated by the responsive output of circular dichroism and circularly polarized luminescence signals of Cu16 moieties of the Cu16@CB8 cluster. Notably, a quantitative chiroptical analysis of amino acids in a short time and a concomitant deracemization of Cu16@CB8 were achieved. Density functional tight-binding molecular dynamics simulation and noncovalent interaction analysis further unraveled the great importance of the cavities and binding sites for chiral recognition. Dipeptide, tripeptide, and polypeptide containing the corresponding amino acids (Cys, Arg, or His residues) display the same chiral recognition, showing the generality of this approach. The functional synergy of dual clusters, comprising carborane and metal clusters, is for the first time demonstrated in the Cu16@CB8 cluster, resulting in the valuable quantification of the enantiomeric excess (ee) value of amino acids. This work opens a new avenue for chirality sensors based on chiral metal clusters with unique chiroptical properties and inspires the development of carborane clusters in host-guest chemistry.

15.
Adv Mater ; 36(30): e2404774, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38721927

ABSTRACT

Green ammonia synthesis through electrocatalytic nitrate reduction reaction (eNO3RR) can serve as an effective alternative to the traditional energy-intensive Haber-Bosch process. However, achieving high Faradaic efficiency (FE) at industrially relevant current density in neutral medium poses significant challenges in eNO3RR. Herein, with the guidance of theoretical calculation, a metallic CoNi-terminated catalyst is successfully designed and constructed on copper foam, which achieves an ammonia FE of up to 100% under industrial-level current density and very low overpotential (-0.15 V versus reversible hydrogen electrode) in a neutral medium. Multiple characterization results have confirmed that the maintained metal atom-terminated surface through interaction with copper atoms plays a crucial role in reducing overpotential and achieving high current density. By constructing a homemade gas stripping and absorption device, the complete conversion process for high-purity ammonium nitrate products is demonstrated, displaying the potential for practical application. This work suggests a sustainable and promising process toward directly converting nitrate-containing pollutant solutions into practical nitrogen fertilizers.

16.
Chem Rev ; 124(11): 7262-7378, 2024 Jun 12.
Article in English | MEDLINE | ID: mdl-38696258

ABSTRACT

Ligand-protected metal clusters possess hybrid properties that seamlessly combine an inorganic core with an organic ligand shell, imparting them exceptional chemical flexibility and unlocking remarkable application potential in diverse fields. Leveraging chemical flexibility to expand the library of available materials and stimulate the development of new functionalities is becoming an increasingly pressing requirement. This Review focuses on the origin of chemical flexibility from the structural analysis, including intra-cluster bonding, inter-cluster interactions, cluster-environments interactions, metal-to-ligand ratios, and thermodynamic effects. In the introduction, we briefly outline the development of metal clusters and explain the differences and commonalities of M(I)/M(I/0) coinage metal clusters. Additionally, we distinguish the bonding characteristics of metal atoms in the inorganic core, which give rise to their distinct chemical flexibility. Section 2 delves into the structural analysis, bonding categories, and thermodynamic theories related to metal clusters. In the following sections 3 to 7, we primarily elucidate the mechanisms that trigger chemical flexibility, the dynamic processes in transformation, the resultant alterations in structure, and the ensuing modifications in physical-chemical properties. Section 8 presents the notable applications that have emerged from utilizing metal clusters and their assemblies. Finally, in section 9, we discuss future challenges and opportunities within this area.

17.
Chem Soc Rev ; 53(13): 6694-6734, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38747082

ABSTRACT

Delayed luminescence (DF), including phosphorescence and thermally activated delayed fluorescence (TADF), and circularly polarized luminescence (CPL) exhibit common and broad application prospects in optoelectronic displays, biological imaging, and encryption. Thus, the combination of delayed luminescence and circularly polarized luminescence is attracting increasing attention. The encapsulation of guest emitters in various host matrices to form host-guest systems has been demonstrated to be an appealing strategy to further enhance and/or modulate their delayed luminescence and circularly polarized luminescence. Compared with conventional liquid crystals, polymers, and supramolecular matrices, porous crystalline frameworks (PCFs) including metal-organic frameworks (MOFs), covalent-organic frameworks (COFs), zeolites and hydrogen-bonded organic frameworks (HOFs) can not only overcome shortcomings such as flexibility and disorder but also achieve the ordered encapsulation of guests and long-term stability of chiral structures, providing new promising host platforms for the development of DF and CPL. In this review, we provide a comprehensive and critical summary of the recent progress in host-guest photochemistry via the encapsulation engineering of guest emitters in PCFs, particularly focusing on delayed luminescence and circularly polarized luminescence. Initially, the general principle of phosphorescence, TADF and CPL, the combination of DF and CPL, and energy transfer processes between host and guests are introduced. Subsequently, we comprehensively discuss the critical factors affecting the encapsulation engineering of guest emitters in PCFs, such as pore structures, the confinement effect, charge and energy transfer between the host and guest, conformational dynamics, and aggregation model of guest emitters. Thereafter, we summarize the effective methods for the preparation of host-guest systems, especially single-crystal-to-single-crystal (SC-SC) transformation and epitaxial growth, which are distinct from conventional methods based on amorphous materials. Then, the recent advancements in host-guest systems based on PCFs for delayed luminescence and circularly polarized luminescence are highlighted. Finally, we present our personal insights into the challenges and future opportunities in this promising field.

18.
Angew Chem Int Ed Engl ; 63(29): e202401724, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38691401

ABSTRACT

The dual emission (DE) characteristics of atomically precise copper nanoclusters (Cu NCs) are of significant theoretical and practical interest. Despite this, the underlying mechanism driving DE in Cu NCs remains elusive, primarily due to the complexities of excited state processes. Herein, a novel [Cu4(PPh3)4(C≡C-p-NH2C6H4)3]PF6 (Cu4) NC, shielded by alkynyl and exhibiting DE, was synthesized. Hydrostatic pressure was applied to Cu4, for the first time, to investigate the mechanism of DE. With increasing pressure, the higher-energy emission peak of Cu4 gradually disappeared, leaving the lower-energy emission peak as the dominant emission. Additionally, the Cu4 crystal exhibited notable piezochromism transitioning from cyan to orange. Angle-dispersive synchrotron X-ray diffraction results revealed that the reduced inter-cluster distances under pressure brought the peripheral ligands closer, leading to the formation of new C-H⋅⋅⋅N and N-H⋅⋅⋅N hydrogen bonds in Cu4. It is proposed that these strengthened hydrogen bond interactions limit the ligands' vibration, resulting in the vanishing of the higher-energy peak. In situ high-pressure Raman and vibrationally resolved emission spectra demonstrated that the benzene ring C=C stretching vibration is the structural source of the DE in Cu4.

19.
Sci Adv ; 10(18): eadn7556, 2024 May 03.
Article in English | MEDLINE | ID: mdl-38691609

ABSTRACT

Atomically precise metal nanoclusters (NCs) are emerging as idealized model catalysts for imprecise metal nanoparticles to unveil their structure-activity relationship. However, the directional synthesis of robust metal NCs with accessible catalytic active sites remains a great challenge. In this work, we achieved bulky carboranealkynyl-protected copper NCs, the monomer Cu13·3PF6 and nido-carboranealkynyl bridged dimer Cu26·4PF6, with fair stability as well as accessible open metal sites step by step through external ligand shell modification and metal-core evolution. Both Cu13·3PF6 and Cu26·4PF6 demonstrate remarkable catalytic activity and selectivity in electrocatalytic nitrate (NO3-) reduction to NH3 reaction, with the dimer Cu26·4PF6 displaying superior performance. The mechanism of this catalytic reaction was elucidated through theoretical computations in conjunction with in situ FTIR spectra. This study not only provides strategies for accessing desired copper NC catalysts but also establishes a platform to uncover the structure-activity relationship of copper NCs.

20.
Angew Chem Int Ed Engl ; 63(34): e202407887, 2024 Aug 19.
Article in English | MEDLINE | ID: mdl-38802322

ABSTRACT

Circularly polarized light (CPL) detection is of great significance in various applications such as drug identification, sensing and imaging. Atomically precise chiral metal nanoclusters with intense circular dichroism (CD) signals are promising candidates for CPL detection, which can further facilitate device miniaturization and integration. Herein, we report the preparation of a pair of optically active chiral silver nanoclusters [Ag7(R/S-DMA)2(dpppy)3] (BF4)3 (R/S-Ag7) for direct CPL detection. The crystal structure and molecular formula of R/S-Ag7 clusters are confirmed by single-crystal X-ray diffraction and high-resolution mass spectrometry. R/S-Ag7 clusters exhibit strong CD spectra and CPL both in solution and solid states. When used as the photoactive materials in photodetectors, R/S-Ag7 enables effective discrimination between left-handed circularly polarized and right-handed circularly polarized light at 520 nm with short response time, high responsivity and considerable discrimination ratio. This study is the first report on using atomically precise chiral metal nanoclusters for CPL detection.

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