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Tin-based sulfides, such as SnS2, have garnered attention as lithium-ion anode materials due to their layer structure and high conductivity capacity. However, during the lithium alloying/dealloying cycles, SnS2 material exhibits a rapid capacity decay due to the volume expansion, which hinders the application of SnS2. In this study, a heterostructure composite material anchored on exfoliated graphite, designated as nano SnS2S3/Sn3S4/FeS/Fe7S8 anchored on 15.0 wt% exfoliated graphite (FSS/G-15%), was synthesized by heating a mixture of inexpensive reducing agent Fe powder and SnS2 powder, followed by ball milling with 15.0 wt% commercial graphite. Experimental results demonstrated that FSS/G-15% had exhibited optimal overall Li+ storage performance, achieving approximately 1306.7, 1199.2, 1033.1, 882.3, 707.3, 507, 366.3, 255.6, and 203.5 mA hg−1 at current densities of 0.1, 0.2, 0.5, 1, 2, 4, 6, 8, and 10 Ag−1, respectively, surpassing the majority of SnS2-based anode materials. The simplicity and efficiency of the synthetic method may have potential implications in various fields in the future. [ABSTRACT FROM AUTHOR]

The burden of premature atherosclerotic cardiovascular disease (ASCVD) has increased rapidly in China. Using the China Health and Nutrition Survey (CHNS) data, we assessed the risk factors of premature ASCVD (age of diagnosis: <55 years for men and <65 years for women). Propensity score matching was used to reduce selection bias. Multivariable Cox proportional-hazards analyses indicated that factors associated with increased risk of premature ASCVD included hypertension (adjusted hazard ratio [HRadj.] = 1.68), obesity (HRadj. = 1.64), and high carbohydrate intake (HRadj. = 1.46). Conversely, participants with medical insurance (HRadj. = 0.42), high urbanization index (HRadj. = 0.53), and high household income (HRadj. = 0.48) had lower risk of premature ASCVD. When comparing premature vs non-premature ASCVD participants, those who were obese (HRadj. = 2.08) or living in more urbanized areas had higher hazards of early onset (HRadj. = 2.29). [ABSTRACT FROM AUTHOR]

The development of efficient, non-toxic, and cost-effective white-light emitters is crucial for advancing lighting technology. Here, we present a groundbreaking study on a new all-inorganic perovskite crystal, CsCaCl3:Mn2+, which exhibits temperature sensing and hue-tunable white light emission. The CsCaCl3 matrix emits broad blue light at 455 nm due to self-trapped exciton (STE) emission. Upon Mn2+ doping, the CsCaCl3:Mn2+ crystal emits broad yellow light at 555 nm, originating from the Mn2+ 4T1(G)–6A1(S) transition. Increasing Mn2+ concentration led to a decrease in blue emission intensity, accompanied by enhanced yellow emission, suggesting an energy transfer from STEs to Mn2+. The enhanced stability of CsCaCl3:Mn2+ compared to pure CsCaCl3 is demonstrated through thermal analysis. The distinctive temperature-dependent responses of STE and Mn2+ emissions in CsCaCl3:Mn2+ suggest its potential application in temperature sensing. The synthesis process for this luminescent crystal is both straightforward and scalable, making it a promising candidate for large-scale applications. [ABSTRACT FROM AUTHOR]

As a new type of negative electrode material for SIBs, (iron germanium sulfide) Fe2GeS4 is considered a highly promising negative electrode material for SIBs owing to its high theoretical capacity, fast Na+ diffusion kinetics, and good thermal stability. In practical applications, it is crucial to synthesize the high-capacity/reversible nanostructured Fe2GeS4-based negative electrodes through an easily executable method. In this study, a two-step synthesis method to prepare nanostructured Fe2GeS4 anchored on graphite (Fe2GeS4/G-15%) was employed: the commercial FeS, S, and Ge powders were mixed and heated, and then graphite was added for ball milling. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that there is a strong interaction between the nanostructured Fe2GeS4 powder and the exfoliated graphite, forming a highly stable nanocomposite material, which is beneficial for improving the reversible charge-discharge performance of the material. When used as a negative electrode material for SIBs, the prepared Fe2GeS4/G-15% exhibited a capacity of 665.5 mAh g−1 during the second cycle at 0.1 A g−1 and could maintain a capacity of 519 mAh g−1 even after the 60th cycle. Considering the simple synthesis process employed in this study, it provides a reference for the production of high-performance Fe2GeS4-based negative electrode materials for SIBs. [ABSTRACT FROM AUTHOR]

Sn-based alloys have emerged as high-capacity, low-working voltage anodes for sodium-ion batteries (SIBs) in recent years, but the complex synthesis processes for highly reversible anodes have impeded their practical application. Herein, DFT calculations demonstrated that SnS2 and Fe can undergo a series of reactions to form Fe–Sn alloys, along with high conductivity/reversible FeSx sulfides. Guided by theoretical calculations, FeS/SnS, FeSn2/FeS/SnS, and FeSn/FeSn2/FeS/SnS heterostructure composites anchored on exfoliated graphite (namely FSS-1/G-15%, FSS-2/G-15%, and FSS-3/G-15%, respectively) were fabricated by annealing Fe and SnS2 mixed powders, and subsequently, ball milling with 15 wt% graphite. Cyclic voltammetry tests, DFT calculations, and ex situ XRD analysis co-confirmed that FeSn and FeSn2 are partially reversible, while FeS and SnS are reversible. FSS-3/G-15% exhibits the best overall Na+-storage performances, which delivered approximately 402, 351, 326, 302, 270, and 259 mA h g−1 at 0.1, 1, 2, 4, 8, and 10 A g−1, with an initial coulombic efficiency of 83.3% at 0.1 A g−1, surpassing most of the recent-reported analogous alloy anodes. The universal material synthesis method only needs one step of thermal reaction, and then ball milling, which may hold great promise in future applications in various fields. [ABSTRACT FROM AUTHOR]

Nickel, cobalt, and manganese oxides are easily obtainable non-noble metal catalysts for water splitting. However, the relationship between composition and catalysts' performance still needs systematic studies. Herein, guided by theoretical calculations, a low overpotential, easily prepared Mn-doped Co3O4 was deposited on graphite plates for water splitting. The 30% Mn-doped Co3O4 (Co2.1Mn0.9O4) required the lowest overpotential for oxygen evolution reaction (OER), in which the Co2.1Mn0.9O4 reached 20, 30, and 50 mA cm−2 in the overpotentials of 425, 451, and 487 mV, respectively, with 90% IR compensation. Under overall water-splitting conditions, the current density reached 30 mA cm−2 at an overpotential of 0.78 V without IR compensation. Charge density difference analysis illustrates that doped Mn provides electrons for O atoms, and that Mn doping also promotes the electron fluctuation of Co atoms. XPS analysis reveals that Mn-doping increases the chemical valence of the Co atom, and that the doped Mn atom also exhibits higher chemical valence than the Mn of Mn3O4, which is advantageous to boost the form of based-OOH* radical, then decrease the overpotential. Considering the particular simplicity of growing the Co2.1Mn0.9O4 on graphite plates, this work is expected to provide a feasible way to develop the high-performance Co-Mn bimetallic oxide for water splitting. [ABSTRACT FROM AUTHOR]

As a unique nanofabrication technology, atomic layer deposition (ALD) has been used in the microelectronics, catalysis, environmental and energy fields. As an energy and catalytic material, nickel sulfide has excellent electrochemical and catalytic activities and has attracted extensive attention. In this work, the reaction mechanism for nickel sulfide ALD from an amidine metal precursor was investigated using density functional theory (DFT) calculations. The results show that the first amidine ligand of bis(N,N′-di-tert-butylacetamidinato)nickel(II) [Ni(tBu-MeAMD)2] can be easily eliminated on the sulfhydrylated surface. The second amidine ligand can also react with the adjacent sulfhydryl group to generate the N,N′-di-tert-butylacetamidine (tBu-MeAMD-H) molecule, which can strongly interact with the Ni atom on the surface and be difficult to be desorbed. In the subsequent H2S reaction, the tBu-MeAMD-H molecule can be exchanged with the H2S precursor. Ultimately, the tBu-MeAMD-H molecule can be desorbed and H2S can be dissociated to form two sulfhydrylated groups on the surface. Meanwhile, the –SH of a H2S molecule can be exchanged with the second tBu-MeAMD ligand. These insights into the reaction mechanism of nickel sulfide ALD can provide theoretical guidance to design the metal amidinate precursors and improve the ALD process for metal sulfides. [ABSTRACT FROM AUTHOR]

Nano-polycrystalline Sn2S3/Sn3S4/FeS/Fe7S8 sulfides anchored on graphene were synthesized via annealing SnS2 and Fe followed by homogeneously combining them with exfoliated graphite. When applied as an anode for a sodium-ion battery, the reversible capacity reached 863 mA h g−1 at 100 mA g−1. This facial materials synthesis method may be applied in various fields. [ABSTRACT FROM AUTHOR]

Porous metal foams (e.g., Ni/Cu/Ti) are applied as catalyst supports extensively for water splitting due to their large specific area and excellent conductivity, however, intrinsic bubble congestion is unavoidable because of the irregular three‐dimensional (3D) networks, resulting in high polarization and degraded electrocatalytic performances. To boost the H2O decomposition kinetics, the immediate bubble removal and water supply sequential in the gas–liquid–solid interface is essential. Inspired by the high efficiency of water/nutrient transport in the capillaries plants, this work designs a graphene‐based capillary array with side holes as catalyst support to manage the bubble release and water supply via a Z‐axis controllable digital light processing (DLP) 3D printing technology. Like planting rice, a low‐cost, high‐active CoNi carbonate hydroxide (CoNiCH) is planted on support. A homemade cell can reach 10 mA cm−2 in 1.51 V, and be kept at 30 mA cm−2 for 60 h without noticeable degradation, surpassing most of the known cells. This research provides a promising avenue to design and prepare advanced catalysts in various fields, including energy applications, pollutant treatment, and chemical synthesis. [ABSTRACT FROM AUTHOR]

As an important inorganic material, zirconium dioxide (ZrO2) has a wide range of applications in the fields of microelectronics, coating, catalysis and energy. Due to its high dielectric constant and thermodynamic stability, ZrO2 can be used as dielectric material to replace traditional silicon dioxide. Currently, ZrO2 dielectric films can be prepared by atomic layer deposition (ALD) using water and zirconium precursors, namely H2O-based ALD. Through density functional theory (DFT) calculations and first-principles molecular dynamics (FPMD) simulations, the adsorption and dissociation of water molecule on the ZrO2 surface and the water–solid interface reaction were investigated. The results showed that the ZrO2 (111) surface has four Lewis acid active sites with different coordination environments for the adsorption and dissociation of water. The Zr atom on the surface can interacted with the O atom of the water molecule via the p orbital of the O atom and the d orbital of the Zr atom. The water molecules could be dissociated via the water–solid interface reaction of the first or second layer of water molecules with the ZrO2 (111) surface. These insights into the adsorption and dissociation of water and the water–solid interface reaction on the ZrO2 surface could also provide a reference for the water–solid interface behavior of metal oxides, such as H2O-based ALD. [ABSTRACT FROM AUTHOR]

This paper studies Chinese grape growers' time discounting and its implications for the adoption of technology that can reduce the negative effects of increasing precipitation. Using primary data collected in Xinjiang Province, we undertook a contingent valuation of rain covers that protect fruit from rain and estimated a discounted utility model using these data. Using a hierarchical Bayesian approach, we find that local grape growers discount the future very heavily, with a discount rate of 0.17 per year, which is almost four times higher than the Chinese market interest rate. Farmers also tend to underestimate the benefits of adopting covers, with their purchase decisions appearing to largely depend on their past actual losses rather than future anticipated losses. These findings have broader implications for policies promoting proactive adaptation in response to likely increased rainfall in the region. Targeting farmers who give lower weight to events far off in the future and understanding that many farmers may tend only to make adoption decisions that have strong short‐term benefits could improve the efficacy of climate policies that target agricultural technologies. [ABSTRACT FROM AUTHOR]

The development of environmentally friendly full‐inorganic luminescent materials with tunable emission properties and exceptional thermal stability is of paramount importance for applications in optoelectronic devices, solid‐state lighting, and anti‐counterfeiting technologies. In this study, a novel luminescent crystal based on calcium perovskites Cs2CaCl4·2H2O (CCCH) are explored using a hydrothermal method. Simultaneous co‐doping of CCCH with Sn2+ and Mn2+ yields the s‐p transition‐induced cyan light from Sn2+ and d‐d transition‐induced yellow light from Mn2+. It demonstrates effective energy transfer from self‐trapped exciton (STE) of matrix CCCH and s‐p transition of Sn2+ to Mn2+, synergizing composite white lights with tunable colors. Furthermore, the incorporation of Sn2+ into CCCH introduces a red shift from blue to cyan emission with a remarkable enhancement in luminescent intensity by a factor of 12 times. The crystal orbital Hamiltonian populations (─COHP) calculations revealed the crucial role of Mn2+ in lattice stability, as evidenced by the decomposition temperature exceeding 305 °C for CCCH:Sn2+,Mn2+ whereas 210 °C for undoped CCCH matrix. This research provides a comprehensive investigation of the luminescent properties of CCCH:Sn2+,Mn2+ crystal, holding significant promise for practical technological advancements in lighting and anti‐counterfeiting technologies. [ABSTRACT FROM AUTHOR]

[Display omitted] • Aluminum precursors bearing alkyl, hydrogen, halide, alkoxy and amino ligands were designed and investigated for Al 2 S 3 atomic layer deposition (ALD). • Amino ligands of aluminum precursors have the self-catalytic role and accelerate the reaction of Al 2 S 3 ALD. • Unlike the concerted elimination of the first amino ligand of aluminum precursors, the elimination of the second amino ligands on the surface is a stepwise process. As a unique nanotechnology, atomic layer deposition (ALD) has been extensively used for the preparation of various nanomaterials. An effective precursor is a prerequisite to ALD success. Herein, we designed and introduced alkyl, hydrogen, halide, alkoxy and amino ligands to aluminum precursors and investigated reaction mechanisms of Al 2 S 3 ALD through density functional calculations. The results show that aluminum precursors with alkyl, hydrogen and halide ligands are kinetically disadvantageous and with alkoxy groups are thermodynamically unfavorable and Al precursors bearing amino groups are thermodynamically and kinetically favorable for Al 2 S 3 ALD. The activity of trimethylaluminum (TMA) on the sulfydrylated surface is lower than that on the hydroxylated surface. The reaction barriers of the aluminum precursors bearing amino ligands on the sulfydrylated surface are obviously lower than that of TMA. Similarly, the barrier of the H 2 S reaction on the aminated surface is much lower than that on the methylated surface. All of the amino groups have a self-catalytic role and accelerate the reaction of Al 2 S 3 ALD. These insights into aluminum precursors bearing amino ligands for Al 2 S 3 ALD can provide theoretical guidance for the discovery of new precursors and the ALD preparation of other aluminum and sulfur compounds. [ABSTRACT FROM AUTHOR]

Electrolysis of water has emerged as a prominent area of research in recent years. As a promising catalyst support, copper foam is widely investigated for electrolytic water, yet the insufficient mechanical strength and corrosion resistance render it less suitable for harsh working conditions. To exploit high-performance catalyst supports, various metal supports are comprehensively evaluated, and Ti 6 Al 4 V (Ti64) support exhibited outstanding compression and corrosion resistance. With this in mind, a 3D porous Ti64 catalyst support is fabricated using the selective laser sintering (SLM) 3D printing technology, and a conductive layer of nickel (Ni) is coated to increase the electrical conductivity and facilitate the deposition of catalysts. Subsequently, Co 0.8 Ni 0.2 (CO 3 ) 0.5 (OH)·0.11H 2 O (CoNiCH) nanoneedles are deposited. The resulting porous Ti64/Ni/CoNiCH electrode displayed an impressive performance in the oxygen evolution reaction (OER) and reached 30 mA cm -2 at an overpotential of only 200 mV. Remarkably, even after being compressed at 15.04 MPa, no obvious structural deformation is observed, and the attenuation of its catalytic efficiency is negligible. Based on the computational analysis, the CoNiCH catalyst demonstrated superior catalytic activity at the Ni site in comparison to the Co site. Furthermore, the electrode reached 30 mA cm -2 at 1.75 V in full water splitting conditions and showed no significant performance degradation even after 60 h of continuous operation. This study presents an innovative approach to robust and corrosion-resistant catalyst design., (© 2024 Wiley-VCH GmbH.)

The quest for efficient and tunable luminescent materials has been at the forefront of research in the fields of chemistry and materials science. This work delves into the investigation of the luminescence properties of Er 3+ ions triggered by 1% Te 4+ in the environmentally benign perovskite Cs 2 NaYbCl 6 (CNYC) crystals, aiming to enhance their efficiency and tune the luminescence color. The ratio of the green ( 2 H 11/2 , 4 S 3/2 - 4 I 15/2 ) to red ( 4 F 9/2 - 4 I 15/2 ) emissions of Er 3+ can be freely tunable by varying the concentration of Er 3+ and producing the defects induced by codoping Te 4+ . The calculations reveal that the multiexcitonic excitations of Er 3+ stem from f-f ( 4 I 15/2 - 4 G 11/2 , 2 H 9/2 ) rather than d-f transitions. The broadened excitation, tuning of color, and enhancement of efficiency achieved in the luminescence perovskite crystals Cs 2 NaYbCl 6 :Te 4+ , Er 3+ (CNYC:Te 4+ ,Er 3+ ) presents promising opportunities for the development of advanced optoelectronic devices with superior performance. Moreover, our investigation demonstrates the tunable luminescence response of CNYC:Er 3+ to temperature variations, offering potential applications in temperature sensing.

Background: Evidence on the association of Olfactory Impairment (OI) with age-related cognitive decline is inconclusive, and the potential influence of allergy remains unclear., Objective: We aimed to evaluate the cross-sectional associations of allergy-related and non-allergy- related OI to cognitive function., Methods: We included 2,499 participants from the Health and Retirement Study (HRS)-Harmonized Cognitive Assessment Protocol (HCAP) sub-study and 1,086 participants from the English Longitudinal Study of Ageing (ELSA)-HCAP. The Olfactory Function Field Exam (OFFE) using Sniffin' Stick odor pens was used to objectively assess olfactory function and an olfactory score <6/11 indicated OI. Mini-Mental Status Examination (MMSE) was used to assess global cognitive function and define cognitive impairment (<24/30). A neuropsychologic battery was used to assess five cognitive domains., Results: Compared to non-OI participants, individuals with OI had lower MMSE z-score [β HRS = -0.33, 95% Confidence Interval (CI): -0.41 to -0.24; β ELSA = -0.31, -0.43 to -0.18] and higher prevalence of cognitive impairment (Prevalence Ratio (PR)HRS = 1.46, 1.06 to 2.01; PR ELSA = 1.63, 1.26 to 2.11). The associations were stronger for non-allergy-related OI (β HRS = -0.36; β ELSA = -0.34) than for allergy-related OI (β HRS = -0.26; β ELSA = 0.13). Similar associations were observed with domain- specific cognitive function measures., Conclusion: OI, particularly non-allergy-related OI, was related to poorer cognitive function in older adults. Although the current cross-sectional study is subject to several limitations, such as reverse causality and residual confounding, the findings will provide insights into the OI-cognition association and enlighten future attention to non-allergy-related OI for the prevention of potential cognitive impairment., (Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.net.)

All-inorganic halide perovskites (AIHPs) have emerged as highly promising optoelectronic materials owing to their remarkable properties, such as high-optical absorption coefficients, photoluminescence efficiencies, and dopant tolerance. Here, we investigate the AIHPs K 4 CdCl 6 :Sb 3+ ,Mn 2+ that demonstrate hue-tunable white-light emission with an exceptional photoluminescence quantum yield of up to 97%. Through a detailed investigation, we reveal that efficient energy transfer from Sb 3+ to Mn 2+ plays a dominant role in the photoluminescence of Mn 2+ , instead of the conventional 4 T 1g → 6 A 1g transition of Mn 2+ . Thermodynamic analysis highlights the crucial role of a Cl-rich environment in obtaining the K 4 CdCl 6 phase, while transformation from K 4 CdCl 6 to KCdCl 3 can be achieved under Cl-poor and K-poor conditions. The theoretical analysis reveals that defect Cl i is more readily formed compared to defect V K , corroborating experimental findings that the K 4 CdCl 6 :Sb 3+ phase is exclusively obtained when the solution contains HCl concentrations higher than 4 mol L -1 . Our work provides valuable insights into the photoluminescence mechanism of Sb 3+ , defect engineering through heterovalent doping, and efficient energy transfer between Sb 3+ and Mn 2+ in K-Cd-Cl-based perovskites, which offers a new perspective for the design and development of novel AIHPs with superior optoelectronic performance.

Antimony (Sb) has been considered a promising anode for sodium-ion batteries (SIBs) owing to its high theoretical capacity (660 mA h g -1 ) and low redox voltage (0.2-0.9 V vs Na + /Na). However, the capacity degradation caused by the volumetric variation during battery discharge/charge hinders the practical application. Herein, guided by the DFT calculation, Sb/Fe 2 S 3 was fabricated by annealing Fe and Sb 2 S 3 mixed powder. Next, Sb/Fe 2 S 3 was blended with 15 wt % graphite by ball milling, yielding nano-Sb/Fe 2 S 3 anchored on an exfoliated graphite composite (denoted as Sb/Fe 2 S 3 -15%). When applied as an anode of SIBs, Sb/Fe 2 S 3 -15% delivered reversible capacities of 565, 542, 467, 366, 285, and 236 mA h g -1 at current rates of 1, 2, 4, 6, 8, and 10 A g -1 , respectively, surpassing most of the Sb-based anodes. The co-existence of highly conductive Fe 2 S 3 and Sb minimizes the polarization of the anode. Our experiments proved that the Sb and Fe 2 S 3 phases were reversible during discharge/charge cycling, and the exfoliated graphite can accelerate the Na + diffusion and e - conduction. The proposed synthesis method of this work can also be applicable to synthesize various antimony/transition metal sulfide heterostructures (Sb/M 1- x S), which may be applied in a series of fields.

As a unique nanofabrication technology, atomic layer deposition (ALD) has been used in the microelectronics, catalysis, environmental and energy fields. As an energy and catalytic material, nickel sulfide has excellent electrochemical and catalytic activities and has attracted extensive attention. In this work, the reaction mechanism for nickel sulfide ALD from an amidine metal precursor was investigated using density functional theory (DFT) calculations. The results show that the first amidine ligand of bis( N , N '-di- tert -butylacetamidinato)nickel(II) [Ni( t Bu-MeAMD) 2 ] can be easily eliminated on the sulfhydrylated surface. The second amidine ligand can also react with the adjacent sulfhydryl group to generate the N , N '-di- tert -butylacetamidine ( t Bu-MeAMD-H) molecule, which can strongly interact with the Ni atom on the surface and be difficult to be desorbed. In the subsequent H 2 S reaction, the t Bu-MeAMD-H molecule can be exchanged with the H 2 S precursor. Ultimately, the t Bu-MeAMD-H molecule can be desorbed and H 2 S can be dissociated to form two sulfhydrylated groups on the surface. Meanwhile, the -SH of a H 2 S molecule can be exchanged with the second t Bu-MeAMD ligand. These insights into the reaction mechanism of nickel sulfide ALD can provide theoretical guidance to design the metal amidinate precursors and improve the ALD process for metal sulfides.

Single-component white light emitters based on the all-inorganic perovskites will act as outstanding candidates for applications in solid-state lighting thanks to their abundant energy states for self-trapped excitons (STE) with ultra-high photoluminescence (PL) efficiency. Here, a complementary white light is realized by dual STEs emissions with blue and yellow colors in a single-component perovskite Cs 2 SnCl 6 :La 3+ microcrystal (MC). The dual emission bands centered at 450 and 560 nm are attributed to the intrinsic STE1 emission in host lattice Cs 2 SnCl 6 and the STE2 emission induced by the heterovalent La 3+ doping, respectively. The hue of the white light can be tunable through energy transfer between the two STEs, the variation of excitation wavelength, and the Sn 4+ /Cs + ratios in starting materials. The effects of the doping heterovalent La 3+ ions on the electronic structure and photophysical properties of the Cs 2 SnCl 6 crystals and the created impurity point defect states are investigated by the chemical potentials calculated using density functional theory (DFT) and confirmed by the experimental results. These results provide a facile approach to gaining novel single-component white light emitter and offer fundamental insights into the defect chemistry in the heterovalent ions doped perovskite luminescent crystals., (© 2023 Wiley-VCH GmbH.)

As a unique nanofabrication technology, atomic layer deposition (ALD) has been widely used for the preparation of various materials in the fields of microelectronics, energy and catalysis. As a high-κ gate dielectric to replace SiO 2 , zirconium oxide (ZrO 2 ) has been prepared through the ALD method for microelectronic devices. In this work, through density functional theory calculations, the possible reaction pathways of ZrO 2 ALD using tetrakis(dimethylamino)zirconium (TDMAZ) and water as the precursors were explored. The whole ZrO 2 ALD reaction could be divided into two sequential reactions, TDMAZ and H 2 O reactions. In the TDMAZ reaction on the hydroxylated surface, the dimethylamino group of TDMAZ could be directly eliminated by substitution and ligand exchange reactions with the hydroxyl group on the surface to form dimethylamine (HN(CH 3 ) 2 ). In the H 2 O reaction with the aminated surface, the reaction process is much more complex than the TDMAZ reaction. These reactions mainly include ligand exchange reactions between the dimethylamino group of TDMAZ and H 2 O and coupling reactions for the formation of the bridged products and the by-product of H 2 O or HN(CH 3 ) 2 . These insights into surface reaction mechanism of ZrO 2 ALD can provide theoretical guidance for the precursor design and improving ALD preparation of other oxides and zirconium compounds, which are based ALD reaction mechanism., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2022 Xu, Zhou, Li, Zhang, Zhu, Xiao, Xu, Ding, Li and Fang.)