Control Of Surface Chemistry Research Articles

(Invited) Low-Temperature Processing of Mixed Conducting Oxides: Control of Defects, Transport, and Reactions Away from Equilibrium

Low-to-intermediate temperature processing and use of mixed conducting oxides targets the following potential benefits: ultra-fine nanostructuring with avoidance of coarsening, control of surface chemistry, lower energy consumption, integration with thermally sensitive components, and slower degradation vs. conventional high temperature synthesis and use. In this lower temperature regime, we have pursued two routes for non-equilibrium control of defect chemistry and therefore properties of mixed ionic/electronic conductors (MIECs) in the ferrite perovskite family: crystallization and illumination.Room-temperature growth followed by mild anneals to induce crystallization has proven to yield superior oxygen surface exchange kinetics, attributed to development of facile charge transfer and pristine surface chemistry in our prior work. The close link between crystallinity and oxygen stoichiometry appears to play an important role in the structural evolution and electrical response. However the effect of evolving crystallinity on the ionic conductivity has not been studied in-depth. Therefore we recently pursued an approach combining in-situ synchrotron grazing-incidence X-ray diffraction with ac and dc electrical methods on thin-film blocking electrode cells to evaluate evolution of transference numbers during crystallization. In certain ferrite films we observe a ~2 orders-of-magnitude increase in ionic conductivity during crystallization, while the electronic conductivity increases much more. Through the process, we demonstrate that it is possible to turn a predominantly ionic conductor into a predominantly electronic conductor - and to access almost any ionic transference number in between - simply by controlling the degree of crystallinity. [1]Oxygen stoichiometry can alternatively be controlled at low-to-intermediate temperatures through application of low fluence above-gap illumination. We have shown in certain non-dilute ferrite films that UV light causes oxygen to enter the films from the gas phase with kinetics limited by the oxygen surface-exchange reaction, which is largely unchanged by the presence of excited carriers. We explain the response through simulations of excited state defect equilibria and transient absorption spectroscopy measurements. [2]Together these processing strategies indicate that low-temperature control of oxygen stoichiometry is feasible in mixed conductors, enabling wide tailoring of properties and potential for use in low-to-intermediate temperature solid-state ionic devices.[1] H.B. Buckner, J. Simpson-Gomez, A. Bonkowski, K. Rubartsch, H. Zhou, R.A. De Souza, N.H. Perry (in review)[2] E. Skiba, H.B. Buckner, G. McKnight, C. Lee, R. Wallick, R. van der Veen, E. Ertekin, N.H. Perry (in review)We gratefully acknowledge funding from the US Department of Energy, Basic Energy Sciences, under DOE Early Career grant DE-SC-0018963 and from the US National Science Foundation, through the University of Illinois at Urbana-Champaign Materials Research Science and Engineering Center DMR-2309037.

(Invited) Electrocatalysis for Complete Aqueous Defluorination of Perfluorooctane Sulfonate

Per- and polyfluoroalkyl substances (PFAS), a group of durable synthetic chemicals widely used in consumer, commercial, and industrial products, have caused global contamination of water, soil, and organisms. Concerns about their persistence and toxicity necessitate advanced remediation strategies. We assessed existing PFAS destruction techniques, emphasizing their limitations such as high costs and energy consumption, and highlighting the need for globally scalable, viable technologies that use nonprecious materials, operate in aqueous media with low energy consumption, and ensure complete PFAS destruction.1 We developed a scalable and economically viable solution using electrocatalysis and ultraviolet light illumination for the mineralization of perfluorooctane sulfonate (PFOS) in aqueous electrolytes with PFOS concentrations as low as 27 ppm, which are environmentally relevant.2 In our approach, we employed pulsed laser in liquids synthesis for the development of nanocatalysts with controlled surface chemistries,3 to facilitate a quantitative mechanistic understanding of electrocatalytic processes, particularly within the electrode microenvironment. Nanosheets of [NiFe]-layered double hydroxide made by pulsed laser in liquid synthesis3,4 were immobilized on hydrophilic carbon fiber paper5 anodes, allowing us to achieve complete defluorination of PFOS in aqueous alkali hydroxide electrolyte.2 Defluorination occurred within the anode microenvironment, as evidenced by pulsed electrolysis vs continuous chronoamperometry data, electrolyte agitation experiments, and XPS data. Importantly, our novel approach uses solely nonprecious materials, and we filed a worldwide patent application for our innovation. Systematic variation of electrocatalysis process parameters provided mechanistic insights into the aqueous defluorination of PFOS.PFAS contamination poses serious threats to humans, ecosystems, water sources, and wildlife. Our newly developed efficient defluorination method is nearly one hundred times cheaper than using boron-doped diamond electrodes and will aid in the remediation of contaminated environments, poised to mitigate the long-term impact of PFAS on aquatic ecosystems, soil quality, and biodiversity. Additionally, lower-income regions globally typically face increased pollution, making electrocatalytic PFAS remediation ideal for decentralized implementation with solar panel-generated electricity, restoring social justice worldwide.2

Revolutionizing applications: the impact of controlled surface chemistry on marble powder.

A large amount of marble powder is abundantly available as a byproduct and waste in the marble industry, and its reinforcement has been attempted in several applications through surface modification. This article examines the use of MP in the production of rubber, paper, foam stabilizers, asphalt, paint, textiles, and adhesives. This article aims to provide a foundation for the surface modification of MP to enhance its properties and broaden its range of applications. Data on modifiers such as organic acids, coupling agents, polymers, and surfactants have been gathered, along with comprehensive reaction details for various techniques, including wet modification, dry modification, in situ modification, ultrasonication, and sol-gel methods. A general overview of MP modification and its impact on composite properties is provided in this review paper, mainly focusing on the distinctive features of composites, contemporary field challenges, and the correlation between the properties and applications of MP.

Ultrathin Copper Monosulfide Films for an Optically Semitransparent, Highly Selective Ammonia Chemosensor.

Transition-metal sulfides are emerging as promising materials for chemiresistive gas sensors─a field still dominated by semiconducting metal oxides. Despite the availability of materials with tunable electronic, optical, physical, and chemical properties, few studies have moved beyond synthesis to provide strategies for enhancing gas sensing performance through material modification. Here, we present a simple, scalable synthetic strategy for developing an optically semitransparent, flexible NH3 gas sensor with a highly uniform, ultrathin CuS (covellite) active sensing layer. The optical and chemical properties of the CuS were precisely controlled near the percolation threshold of thin-film formation by varying key experimental parameters such as the Cu film thickness (<10 nm) and the sulfurization time (∼90 s) under ambient conditions. Experimental and computational studies of CuS and its NH3 sensing characteristics identify key physicochemical properties. The controlled surface chemistry and morphology of the ultrathin CuS layer demonstrate its effectiveness in functional NH3 sensing devices, which achieve a calculated detection limit of 1.38 ppm for NH3 gas at 150 °C, along with exceptional mechanical robustness and optical semitransparency in the visible-light spectrum.

Non-Invasive Disposable 2D Ti3C2Tx based Enzyme Free Electrochemical Sweat Glucose Biosensor

Modern analytical chemistry, enhanced by advancements in materials science, is crucial for cost-effectively improving measurement techniques, and making analyses more accessible and user-friendly. Disposable screen-printed electrodes have emerged as promising tools, offering miniaturization, high reproducibility, high sensitivity, rapid detection, and inherent selectivity. This study highlights the development of advanced 2D Ti3C2Tx MXene-modified disposable screen-printed gold electrodes for non-invasive, enzyme-free glucose sensing. Ti3C2Tx was synthesized using direct and in-situ etchants to achieve controlled surface chemistry. Techniques such as XRD, UV–visible spectroscopy, SEM, and TEM were employed to characterize Ti3C2Tx synthesized with different etchants. The synthesized materials were then used as working electrodes to investigate their electrocatalytic performance, tailored for continuous glucose monitoring. Upon optimization, in-situ LiF and HCl etched Li-Ti3C2Tx@SPGE exhibited a high sensitivity of 569.70 µA mM−1cm−2, followed by HF-Ti3C2Tx@SPGE and N-Ti3C2Tx@SPGE with sensitivities of 249.62 and 297.78 µA mM−1cm−2, respectively. These sensors demonstrated low limits of detection (LOD) of 5 nM, 28 nM, and 19 nM within a linear range of 5 to 350 µM. Additionally, real sweat analysis was conducted by collecting natural sweat through fast walking and evaluating sensor performance after beverage consumption. Overall, Li-Ti3C2Tx@SPGE, without any additional composition or doping, shows potential as a superior commercial sweat sensor for routine glucose monitoring. This study underscores the innovative use of 2D materials in developing highly sensitive, non-invasive sweat glucose sensors that are both effective and accessible.

Controlling surface chemistry in cold sintering to advance battery materials

Cold sintering is a recently introduced densification method that is of interest due to the lower energy used in the process, the ability to densify metastable materials, the ability to integrate materials to develop unique composites, and the ability to synthesis materials that can be more easily recycled. Collectively, these advantages make cold sintering a promising approach for processing of battery components, and co-sintering into all solid-state batteries. To obtain high electrochemical performance with cold sintering, detailed control of the surface chemistry of powders is needed, to avoid or minimize the impact of carbonate formation in grain boundaries, and to limit concentrations of secondary phases that are a result of incongruent dissolution processes. In this paper, we outline the importance of surface chemical reactions of powders in cold sintering, and the mitigating processes that can be adopted to control these reactions and obtain high performance and unique opportunities for Li and Na-oxide secondary batteries. We focus on a series of examples that demonstrate how the control of low temperature densification (cold sintering) can address the environmental sensitivity of many battery materials, and highlight the issues faced and open questions. These examples include cold sintering of air-sensitive solid electrolytes, re-processing of crushed solid electrolytes, surface passivation of air-sensitive active materials for processing in air, and fabrication of solid-solid macroscopic interfaces for solid-state batteries.

Insight into the mechanism of nitrogen doping in MXenes with controllable surface chemistry

Nitrogen doping emerges as a potent strategy to enhance the electrochemical attributes of two-dimensional MXene materials, recognized for their utility in energy storage solutions. Although advancements have been made, the specific roles of varied doping sites in modifying electrochemical behavior are not fully delineated. This investigation explores nitrogen-doping mechanisms in MXenes with tailored surface chemistries, utilizing a blend of experimental approaches and density functional theory calculations. The distinct roles of nitrogen dopant sites are explored, and the evolution of the electronic structure and stability of the material before and after nitrogen modifications via the urea hydrothermal method are also investigated. The synthesized N-V2CTx-160 MXene electrodes exhibit favorable surface characteristics for energy storage, achieving impressive capacitance properties with a gravimetric capacitance of 592.9 F/g at 2 mV/s in 1 M H2SO4 electrolyte. This work provides a valuable insight for the development of high-performance MXene electrodes for energy storage applications.

Constructing surface protective film of V-Se-O to promote zinc ion storage by surface oxygen implantation strategy

Interfacial chemical modification is an effective strategy to adjust the strong Coulombic ion-lattice interactions with high valence cations experienced by electrode materials, facilitating the reaction kinetic. In this paper, a simple and fast surface oxygen implantation strategy was designed to adjust the electronic structure of stainless steel (SS) supported vanadium diselenide (VSe2) nanosheets and form a surface protective film, which effectively accelerates the reaction kinetics of Zn2+ and extends the cycle life of the battery. It is demonstrated that the conductivity, pseudocapacitance and specific capacity can be tuned by selectively introducing oxygen species to the surface, which provides an important reference for the design of electrodes with controlled surface chemistry. Density functional theory (DFT) calculations also confirm that the electronic structure can be adjusted by surface oxygen injection strategy, which not only improves the conductivity, but also adjusts the adsorption energy, thus providing favorable conditions for zinc ion storage. Benefiting from the selenium vacancies and pores generated by the removal of part of selenium, and the oxide film formed on the surfaces, the VSe2-xOx-SS-30 electrode showed higher specific capacity (188.4 mAh/g at 0.5 A g−1 after 50 cycles), better rate performance (107.1 mAh/g at 4 A g−1) and more satisfactory cycling stability (83.1 mAh/g at 5 A g−1 after 1800 cycles) than VSe2-SS electrode. Importantly, the flexible quasi-solid-state VSe2-xOx-SS-30//Zn battery also exhibits high specific capacity and excellent environmental adaptability. Furthermore, the zinc (de)intercalation and transformation reactions mechanism was revealed by some ex-situ/in-situ techniques.

Delaying frost formation by controlling surface chemistry of ZnO-coated 304 stainless steel surfaces

Because 304 stainless steel is extensively used in everyday life, surface icing frost would cause annoyance; thus, the research on 304 stainless steel with frost inhibition is quite important. The superhydrophobic surface anti-frost is energy-saving and ecologically beneficial, but it also avoids typical defrosting, which reduces energy consumption, pollution, and other difficulties. As a result, the investigation of superhydrophobic surface frost inhibition performance offers promising practical potential. However, traditional manufacturing procedures for superhydrophobic surfaces have proven to be difficult and expensive, rendering them unsuitable for mass production. In this paper, a simple hydrothermal and sol-gel method were used to prepare the superhydrophobic surface wettability of 304 stainless steel and determine the frosting behavior of superhydrophobic ZnO, hydrophobic ZnO, hydrophilic ZnO, and 304 stainless steel sheets at low ambient temperatures. The frost resistance of superhydrophobic ZnO was studied. As a result, this study provides a novel idea for rationally designing frost-resistant superhydrophobic surfaces at low ambient temperatures.

Phenylacetylene-Terminated Poly(Ethylene Glycol) as Ligands for Colloidal Noble Metal Nanoparticles: a New Tool for "Grafting to" Approach.

We report a new design of polymer phenylacetylene (PA) ligands and the ligand exchange methodology for colloidal noble metal nanoparticles (NPs). PA-terminated poly(ethylene glycol) (PEG) can bind to metal NPs through acetylide (M-C≡C-R) that affords a high grafting density. The ligand-metal interaction can be switched between σ bonding and extended π backbonding by changing grafting conditions. The σ bonding of PEG-PA with NPs is strong and it can compete with other capping ligands including thiols, while the π backbonding is much weaker. The σ bonding is also demonstrated to improve the catalytic performance of Pd for ethanol oxidation and prevent surface absorption of the reaction intermediates. Those unique binding characteristics will enrich the toolbox in the control of colloidal surface chemistry and their applications using polymer ligands.

Control of Surface Chemistry in Recess Etching toward Normally Off GaN Metal–Insulator–Semiconductor High‐Electron‐Mobility Transistors

Reducing off‐state and gate leakage current is crucial in the development of metal–insulator–semiconductor high‐electron‐mobility transistors (MIS‐HEMTs). This work reports interface engineering in the gate recess region through low‐damage digital etching during the fabrication of normally off GaN MIS‐HEMTs. Conventional plasma etching leads to a reduction of the N/(Al+Ga) ratio, but this value recovers to almost 1 with optimized oxidation condition during digital etching, suggesting a reduction of the Al/Ga dangling bonds based on the proposed technique. GaN MIS‐HEMTs with digital etching exhibits a threshold voltage of 1.0 V at 1 μA mm−1, a high ON/OFF current ratio of 1010, a gate breakdown voltage of 22 V, and a low gate leakage current of 10−8 mA mm−1.

Adsorption and Structuration of PEG Thin Films: Influence of the Substrate Chemistry.

This study investigates polyethylene glycol (PEG) homopolymer thin film adsorption on gold surfaces of controlled surface chemistry. The conformational states of physisorbed PEG are analyzed through polarization modulation infrared reflection-absorption spectrometry (PM-IRRAS). The PM-IRRAS principle is based on specific optical selection rules allowing the detection of surface-specific FTIR response of thin polymer films on the basis of differential reflectivity at the polymer/substrate interface for p- and s-polarized light. The intensification of the electric field generated at the PEG/substrate interface for p-polarized IR light in comparison with s-polarized light permits the analysis of PEG chain anisotropy and conformational changes induced by the adsorption. Results showed that PEG adsorbs on model substrates having a rather hydrophilic character in a way that the PEG chains spread parallel to the surface. In the case of a very hydrophilic substrate, the adsorbed PEG chains are in a stable thermodynamic state which allows them to arrange and crystallize as stacked crystalline lamellae after adsorption. The surface topography and morphology of the PEG thin films were also investigated by atomic force microscopy (AFM). While in the bulk state, PEG crystallizes in the form of large spherulites; on substrates whose adsorption is favored by surface chemistry, PEG crystallizes in the form of stacked lamellae with a thickness equal to 20 nm. Conversely, on a hydrophobic substrate, the PEG chains do not crystallize and adsorption occurs in the statistical coil state.

Tuning the Surface Stability and Li/Na Storage of MXenes by Controlling the Surface Termination Coverage.

2D transition metal carbides and/or nitrides, MXenes, are a class of widely studied materials with great potential for energy storage applications. The control of surface chemistry is an effective approach for preparing novel MXenes and modifying their electrochemical properties. However, an in-depth and systematic atomic-scale study of the effect of surface termination on MXene stability and electrochemical performance is scarce and thus is highly desired. Here, through high-throughput first-principles calculations, 28 stable chalcogen-functionalized M2CTz (M = V, Nb, and Ta, T = S, Se, and Te) under different chemical environments are identified. The reduction of termination coverage improves electrical conductivity but weakens in-plane stiffness. Intriguingly, based on charge transfer mechanism, the diffusion barrier of lithium/sodium atoms on the M2CTz exhibits a volcano-like relationship with termination coverage, and the ion diffusion channel formed in half termination coverage greatly accelerates lithium ion diffusion and returns to or exceeds sodium ion diffusion rate at full termination coverage. V2CSe2/Nb2CSz not only displays the large lithium/sodium capacity (592/409-466 mAhg-1) but also exhibits low barrier energy and open-circuit voltage, suggesting a promising candidate anode material for lithium/sodium-ion batteries. These findings provide insights into the design and fabrication of MXenes and tuning the electrochemical performance of MXenes by controlling termination coverage.

Advanced polymeric dendrimers in the management of Alzheimer's disease

AbstractIn recent years, advanced polymeric dendrimers have emerged as a promising avenue for AD management. Dendrimers are highly branched, three‐dimensional macromolecules with precise nanoarchitectures, making them ideal candidates for the delivery of therapeutic agents and diagnostic tools. Their unique properties, such as well‐defined size, multifunctionality, and controlled surface chemistry, allow for the design of targeted and highly efficient drug delivery systems and diagnostic probes. This review aims to provide a comprehensive overview of the potential applications of advanced polymeric dendrimers in the management of Alzheimer's disease. We explored their role in drug delivery, diagnostics, and other therapeutic interventions for AD. Additionally, we will delve into the challenges and opportunities in utilizing dendrimers as a key player in the battle against this devastating disease. The review will begin by discussing the current state of Alzheimer's disease, including its pathological features, clinical manifestations, and existing treatment strategies. It will then transition to an in‐depth examination of polymeric dendrimers, highlighting their structural characteristics, synthesis methods, and biocompatibility. Subsequently, the review will delve into the various ways in which dendrimers can be tailored for AD management, including drug encapsulation and delivery, enhanced blood–brain barrier penetration, and targeted diagnostic imaging. Furthermore, we explored the potential benefits of dendrimer‐based therapies, such as improved drug efficacy, reduced side effects, and enhanced patient compliance. The review will also address the challenges associated with dendrimer‐based approaches, including toxicity concerns, regulatory hurdles, and the need for rigorous clinical evaluation.

Synthesis of Hierarchical Superhydrophilic/Superhydrophobic Nanostructured Surfaces for Oil/Water Separation

AbstractSurface wetting, the phenomenon where a liquid spreads or adheres to a solid surface, plays a crucial role in both natural and technological fields. This study focuses on elucidating the relationship between surface properties and wetting behavior, emphasizing the significance of hierarchical structures. A 3D hierarchical structure is created by controlling shape and size through electroplating and chemical reactions, adjusted by current intensity, ammonium persulfate, and ammonium hydroxide concentrations. This modification is achieved by modifying the surface's chemical properties. This control directly impacted the surface wetting properties, providing a means to regulate wetting behavior by altering surface structure. Through control of surface chemistry, a superhydrophilic surface is able to successfully create with a contact angle of 0° and a superhydrophobic surface with a contact angle of 171.3.

Targeted synthesis of gold nanorods and characterization of their tailored surface properties using optical and X-ray spectroscopy.

In recent years, nanophotonics have had a transformative impact on harnessing energy, directing chemical reactions, and enabling novel molecular dynamics for thermodynamically intensive applications. Plasmonic nanoparticles have emerged as a tool for confining light on nanometer-length scales where regions of intense electromagnetic fields can be precisely tuned for controlled surface chemistry. We demonstrate a precision pH-driven synthesis of gold nanorods with optical resonance properties widely tunable across the near-infrared spectrum. Through controlled electrostatic interactions, we can perform selective adsorbate molecule attachment and monitor the surface transitions through spectroscopic techniques that include ground-state absorption spectrophotometry, two-dimensional X-ray absorption near-edge spectroscopy, Fourier-transform infrared spectroscopy, and surface-enhanced Raman spectroscopy. We elucidate the electronic, structural, and chemical factors that contribute to plasmon-molecule dynamics at the nanoscale with broad implications for the fields of energy, photonics, and bio-inspired materials.

Versatile MXenes for Aqueous Zinc Batteries.

Aqueous zinc-ion batteries (AZIBs) are gaining popularity for their cost-effectiveness, safety, and utilization of abundant resources. MXenes, which possess outstanding conductivity, controllable surface chemistry, and structural adaptability, are widely recognized as a highly versatile platform for AZIBs. MXenes offer a unique set of functions for AZIBs, yet their significance has not been systematically recognized and summarized. This review article provides an up-to-date overview of MXenes-based electrode materials for AZIBs, with a focus on the unique functions of MXenes in these materials. The discussion starts with MXenes and their derivatives on the cathode side, where they serve as a 2D conductive substrate, 3D framework, flexible support, and coating layer. MXenes can act as both the active material and a precursor to the active material in the cathode. On the anode side, the functions of MXenes include active material host, zinc metal surface protection, electrolyte additive, and separator modification. The review also highlights technical challenges and key hurdles that MXenes currently face in AZIBs.

Modulating pro-adhesive nature of metallic surfaces through a polypeptide coupling via diazonium chemistry

The design of biomaterials able to facilitate cell adhesion is critical in the field of tissue engineering. Precise control of surface chemistry at the material/tissue interface plays a major role in enhancing the interactions between a biomaterial and living cells. Bio-integration is particularly important in case of various electrotherapies, since a close contact between tissue and electrode's surface facilitates treatment. A promising approach towards surface biofunctionalization involves the electrografting of diazonium salts followed by the modification of organic layer with pro-adhesive polypeptides. This study focuses on the modification of platinum electrodes with a 4-nitrobenzenediazonium layer, which is then converted to the aminobenzene moiety. The electrodes are further biofunctionalized with polypeptides (polylysine and polylysine/laminin) to enhance cell adhesion. This study also explores the differences between physical and chemical coupling of selected polypeptides to modulate pro-adhesive nature of Pt electrodes with respect to human neuroblastoma SH-SY5Y cells and U87 astrocytes. Our results demonstrate the significant enhancement in cell adhesion for biofunctionalized electrodes, with more amplified adhesion noted for covalently coupled polypeptides. The implications of this research are crucial for the development of more effective and functional biomaterials, particularly biomedical electrodes, which have the potential to advance the field of bioelectronics and improve patients' outcomes.

Nanodelivery Systems as a Novel Strategy to Overcome Treatment Failure of Cancer.

Despite the tremendous progress in cancer treatment in recent decades, cancers often become resistant due to multiple mechanisms, such as intrinsic or acquired multidrug resistance, which leads to unsatisfactory treatment effects or accompanying metastasis and recurrence, ultimately to treatment failure. With a deeper understanding of the molecular mechanisms of tumors, researchers have realized that treatment designs targeting tumor resistance mechanisms would be a promising strategy to break the therapeutic deadlock. Nanodelivery systems have excellent physicochemical properties, including highly efficient tissue-specific delivery, substantial specific surface area, and controllable surface chemistry, which endow nanodelivery systems with capabilities such as precise targeting, deep penetration, responsive drug release, multidrug codelivery, and multimodal synergy, which are currently widely used in biomedical researches and bring a new dawn for overcoming cancer resistance. Based on the mechanisms of tumor therapeutic resistance, this review summarizes the research progress of nanodelivery systems for overcoming tumor resistance to improve therapeutic efficacy in recent years and offers prospects and challenges of the application of nanodelivery systems for overcoming cancer resistance.

Mild and Efficient Method for the In Situ Preparation of High‐Quality MXene Materials Enabled by Hexafluoro Complex Anion Contained Salts Etching

AbstractMXene is a promising two‐dimensional (2D) material for energy storage applications owing to its exceptional conductivity and controllable surface chemistry. Currently, aqueous etching methods for the preparation of MXene sheets require a substantial quantity of HF or HCl, leading to issues such as structural defects in the MXene sheets and severe corrosiveness due to the acidic nature of these etchants. This study proposes a mild in situ etching strategy for the preparation of MXene materials through hexafluoro complex anion hydrolysis etching. Etching is accomplished by gradually introducing water into a suspension composed of hexafluoro complex, ethanol, and Ti3AlC2. This process results in the production of high‐quality MXene in a mild reaction environment with the weak acidity of the solution, making it suitable for scalable synthesis and process applications. Moreover, the inclusion of ethanol in the etching process increases the interlamellar spacing of MXene, thereby facilitating the stripping process and ultimately yielding of 28% in the production of single‐layer MXene through shaking. The MXene incorporated into the Si/C anode demonstrates a notable reversible cycling capacity of 563 mAh g−1 after 120 cycles, accompanied by an initial coulombic efficiency (CE) of 83%, surpassing the performance of Si/C anodes modified with carbon nanotubes (CNTs) and Super P. The approach presented in this study offers a promising pathway for the safe, straightforward, and sustainable production of high‐quality MXene materials.