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Multimetallic nanoclusters (MMNCs) offer unique and tailorable surface chemistries that hold great potential for numerous catalytic applications. The efficient exploration of this vast chemical space necessitates an accelerated discovery pipeline that supersedes traditional “trial-and-error” experimentation while guaranteeing uniform microstructures despite compositional complexity. Herein, we report the high-throughput synthesis of an extensive series of ultrafine and homogeneous alloy MMNCs, achieved by 1) a flexible compositional design by formulation in the precursor solution phase and 2) the ultrafast synthesis of alloy MMNCs using thermal shock heating (i.e., ∼1,650 K, ∼500 ms). This approach is remarkably facile and easily accessible compared to conventional vapor-phase deposition, and the particle size and structural uniformity enable comparative studies across compositionally different MMNCs. Rapid electrochemical screening is demonstrated by using a scanning droplet cell, enabling us to discover two promising electrocatalysts, which we subsequently validated using a rotating disk setup. This demonstrated high-throughput material discovery pipeline presents a paradigm for facile and accelerated exploration of MMNCs for a broad range of applications.

Exploring intermetallic synergy has allowed a series of alloy nanoparticles with prominent chemical–physical properties to be produced. However, precise alloying based on a maintained template has long been a challenging pursuit, and little has been achieved for manipulation at the atomic level. Here, a nanosystem based on M29(S-Adm)18(PPh₃)₄ (where S-Adm is the adamantane mercaptan and M is Ag/Cu/Au/Pt/Pd) has been established, which leads to the atomically precise operation on each site in this M29 template. Specifically, a library of 21 species of nanoclusters ranging from monometallic to tetrametallic constitutions has been successfully prepared step by step with in situ synthesis, target metal-exchange, and forced metal-exchange methods. More importantly, owing to the monodispersity of each nanocluster in this M29 library, the synergetic effects on the optical properties and stability have been mapped out. This nanocluster methodology not only provides fundamental principles to produce alloy nanoclusters with multimetallic compositions and monodispersed dopants but also provides an intriguing nanomodel that enables us to grasp the intermetallic synergy at the atomic level.

Understanding the interaction of nanomaterials with biological systems has always been of high concern and interest. An emerging type of nanomaterials, ultrasmall metal nanoclusters (NCs, < 2 nm in size), are promising in this aspect due to their well-defined molecular formulae and structures, as well as unique physical and chemical properties that are distinctly different from their larger counterparts (metal nanoparticles). For example, metal NCs possess intrinsic strong luminescence, which can be used for real-time tracking of their interactions with biological systems. Herein, luminescent gold (Au) NCs were used as traceable antimicrobial agents to study their interactions with the bacteria and to further understand their underlining antimicrobial mechanism. It is shown for the first time that the Au NCs would first attach on the bacterial membrane, penetrate, and subsequently accumulate inside the bacteria. Thereafter, the internalized Au NCs would induce reactive oxygen species (ROS) generation and damage the bacterial membrane, resulting in the leakage of bacterial contents, which can finally kill the bacteria. Traceable Au NCs (or other metal NCs) provide a promising platform to study the antimicrobial mechanisms as well as other fundamentals on the interfacing of functional nanomaterials with the biological systems, further increasing their acceptance in various biomedical applications.

Aggregation-induced emission (AIE) is an intriguing strategy to enhance the luminescence of metal nanoclusters (NCs). However, the morphologies of aggregated NCs are often irregular and inhomogeneous, leading to instability and poor color purity of the aggregations, which greatly limit their further potential in optical applications. Inspired by self-assembly techniques, manipulating metal NCs into well-defined architectures has achieved success. The self-assembled metal NCs often exhibit enhancing emission stability and intensity compared to the individually or randomly aggregated ones. Meanwhile, the emission color of metal NCs becomes tunable. In this review, we summarize the synthetic strategies involved in self-assembly of metal NCs for the first time. For each synthetic strategy, we describe the self-assembly mechanisms involved and the dependence of optical properties on the self-assembly. Finally, we outline the current challenges to and perspectives on the development of this area.

Owing to their remarkable properties, gold nanoparticles are applied in diverse fields, including catalysis, electronics, energy conversion and sensors. However, for catalytic applications of colloidal gold nanoparticles, the trade-off between their reactivity and stability is a significant concern. Here we report a universal approach for preparing stable and reactive colloidal small (~3 nm) gold nanoparticles by using multi-dentate polyoxometalates as protecting agents in non-polar solvents. These nanoparticles exhibit exceptional stability even under conditions of high concentration, long-term storage, heating and addition of bases. Moreover, they display excellent catalytic performance in various oxidation reactions of organic substrates using molecular oxygen as the sole oxidant. Our findings highlight the ability of inorganic multi-dentate ligands with structural stability and robust steric and electronic effects to confer stability and reactivity upon gold nanoparticles. This approach can be extended to prepare metal nanoparticles other than gold, enabling the design of novel nanomaterials with promising applications. For catalytic nanoparticles there is often a trade-off between stability and activity. Here the authors report a route to ultra-stable and catalytically active colloidal small (~3 nm) gold nanoparticles using multi-dentate polyoxometalates as protecting agents in nonpolar solvents.

Electrocatalytic nitrate reduction reaction (NO 3 RR) offers a unique rationale for green NH 3 synthesis, yet the lack of high-efficiency NO 3 RR catalysts remains a great challenge. In this work, we show that Au nanoclusters anchored on TiO 2 nanosheets can efficiently catalyze the conversion of NO 3 RR-to-NH 3 under ambient conditions, achieving a maximal Faradic efficiency of 91%, a peak yield rate of 1923 µg·h −1 ·mg cat. −1 , and high durability over 10 consecutive cycles, all of which are comparable to the recently reported metrics (including transition metal and noble metal-based catalysts) and exceed those of pristine TiO 2 . Moreover, a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed, which shows a power density of 3.62 mW·cm −2 and a yield rate of 452 µg·h −1 ·mg cat. −1 . Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO 3 − species, and reduce the NO 3 RR-to-NH 3 barrier, thus leading to an accelerated cathodic reaction. This work highlights the importance of metal clusters for the NH 3 electrosynthesis and nitrate removal.

In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3–3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20–54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)−1 in a roadside environment, 2.6·1015 (kgfuel)−1 in a street canyon, and 2.9·1015 (kgfuel)−1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)−1 to a high value of 4.3·1015 (kgfuel)−1. These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Chiral nanomaterials have recently stimulated significant interest in both fundamental research and practical applications (e.g., nanoprobes for biomolecular recognition). However, achieving chiral nanoclusters is still a major challenge. Herein, we report an effective strategy that affords achiral diphosphine ligand‐protected, chiral Au11 nanoclusters. Synchrotron radiation X‐ray diffraction solves the chiral structure of Au11(dppp)5Cl3 (dppp = 1,3‐bis(diphenylphosphino)propane) and further reveals that the critical feature of bidentate binding of diphosphine induces the unique ansa‐metallamacrocycle pattern (i.e., the “Au─P─CH2CH2CH2─P─Au” staple). All the possible ansa‐metallamacrocycle patterns are transferred to the most robust pattern by “ligand confinement,” giving rise to the chiral enantiomers. Using Density Functional Theory (DFT), we show that the chirality can emerge due to the low energy barriers facilitating the transformation of the symmetric Au11 core into the corresponding asymmetric chiral cluster, driven by a favorable fit of ligand bridges. This new type of chiral nanomaterial holds promise in chiral sensing/recognition and enantioselective applications. In this work, we prepare a chiral Au11 nanocluster ligated by diphosphine ligand, Au11(dppp)5Cl3, which is induced by the unique ansa‐metallamacrocycle stain (the “Au─P─CH2CH2CH2─P─Au” staple).

In the clinical diagnosis of tumors, a single-marker immunoassay may lead to false results. Thus there is a need for an effective and valid method for the simultaneous measurement of multiple tumor markers. In this work, an efficient fluorescence immunosensor for the simultaneous measurement of CA125 and CA15–3 tumor markers was fabricated by utilizing the high selectivity of magnetic molecularly imprinted polymers (MMIPs) and the high sensitivity of a fluorescence (FL) method. Ni nanoclusters (Ni NCs) and noble Cd nanoclusters (Cd NCs) were introduced as efficient and economic emitters, and magnetic graphene oxide (GO–Fe3O4) was applied as a support material for surface molecularly imprinted polymers. Under the most favorable experimental conditions, the fluorescence intensity of the Cd NCs and Ni NCs gradually increased with increasing concentration of CA125 and CA15–3 antigens at a range of 0.0005–40 U mL−1, respectively, with a limit of detection (LOD) of 50 μU mL−1. The developed method had excellent properties including a broad linear range, good reproducibility, and simple operation for the clinical diagnosis of CA 125 and CA 15–3 tumor markers. This molecularly imprinted fluorescence sensor has the potential to be an effective clinical tool for the timely screening of breast cancer in human serum samples and OVCAR-3 and MCF-7 cell lines, and can be applied in clinical diagnostics.