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C. Chen

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15 records found

Machine learning–accelerated computations combined with experiments

Journal article (2026) - Jiawei Tang, Weiwei Sun, Chaofan Chen, Lars Bannenberg, Xuehang Wang, Tingwei Zhu, Litao Sun, Jinlan Wang, Yu Xie, More Authors
Nanoconfined water exhibits unique properties compared to bulk water due to limited quantities, frustrated hydrogen bonding, and surface interactions, which are fundamental for energy storage and transport applications. We integrate machine learning–accelerated ab initio molecular dynamics with x-ray diffraction (XRD) and inelastic neutron scattering (INS) to systematically analyze the thermodynamic and dynamic behavior of water confined between functionalized (-F, -O, and -OH) two-dimensional (2D) Ti3C2Tx MXene layers. As water intercalates between layers, the interlayer spacing exhibits layer-dependent staging characteristics. The water polarization can be flipped by the count and morphology of intercalated molecules interacting with MXene surface groups, resulting in varying electrostatic potential profiles. On the basis of interfacial electrostatic potential, hydrogen bond lifetime, and molecular orientation, we establish a linear combination of exponential model describing water diffusivity. These computational insights align well with experimental x-ray and neutron measurements, suggesting strategies for tuning water morphology and transport by tailoring MXene surface chemistry and water content for electrochemical energy storage and nanofluidic applications. ...
Doctoral thesis (2026) - C. Chen, M. Wagemaker, Xuehang Wang
This thesis aims to help understand how ion solvation influences the charge storage behavior of Ti3C2Tx MXene in neutral aqueous electrolytes. This is achieved through two main approaches. First, electrolyte engineering strategy has been employed to tune ion solvation structures through varying ion species and solvents. This enables control over the intercalation behavior of both non-metallic and metallic ions into MXene’s interlayer, as well as the deposition behavior of Zn2+ ions on Ti3C2Tx surface. Second, the electrode architecture is modified by constructing a redox-active Ti3C2Tx/conjugated polyelectrolyte (CPE) heterostructure. This design alters the local interlayer environment and influences the desolvation behavior of ammonium ions.

The thesis is organized into three parts, the first part of this thesis focuses on the intercalation of non-metallic ions into Ti3C2Tx, starting with a systematic study on ammonium (NH4⁺) and tetraalkylammonium ions (TMA⁺, TEA⁺, and TPA⁺) intercalation (chapter 2). These ions, with distinct sizes and solvation structures, provide a platform to understand how solvation influences non-metallic ion storage behavior of flexible 2D materials. Considering the moderate capacitance of Ti3C2Tx for ammonium ion storage, we designed a redox-active heterostructure composed of Ti3C2Tx and a n-type cationic conjugated polyelectrolytes (CPE) (chapter 3). In this chapter, we found that structural tuning at the electrode level can affect ion desolvation, which in turn affects the charge storage behavior.

The second part of the thesis investigates how electrolyte design can be used to control ion solvation structures, with the goal of tuning metallic ion intercalation behavior in Ti3C2Tx. In chapter 4, polyethylene glycol (PEG-400) is introduced as a molecular crowding agent in Li⁺-based aqueous electrolytes. This modification extends the voltage window and tunes the Li+ intercalation behavior at higher potential. In chapter 5, acetonitrile (ACN) was used as co-solvent to tune the solvation environment of Na⁺ ions. By varying the ACN content, the strength of ion-solvent interactions is adjusted, leading to change in charge storage mechanism and electrochemical performance. The third part (chapter 6) examines how ion solvation affects Zn²⁺ deposition behavior on Ti3C2Tx, which is used as a freestanding current collector in anode-free aqueous zinc metal batteries (AZMBs). By introducing Li-salts and propylene carbonate (PC) as electrolyte additives, the solvation structure of Zn²⁺ ions is altered, which directly influences interfacial chemistry at the MXene surface. This modulation leads to the formation of a ZnF2-rich interphase that stabilizes Zn deposition and improves cycling efficiency. These findings demonstrate how tailoring ion solvation can serve as a powerful strategy to control not only intercalation, but also metal deposition behavior in MXene-based charge storage systems. ...
Review (2026) - Jiali Tang, Chao Chen, Bo Wang, Changjun Li, Jie Li, Ming Yang, Ernesto Salzano
Rising concerns over carbon emissions from fossil fuels have fueled interest in renewable energies. Hydrogen, as a clean energy source, stands out for its free of pollution and high calorific value. However, challenges in safely storing and transporting hydrogen, such as embrittlement, fire and explosion risks, are critical. This study reviews hydrogen storage and transportation safety research through a bibliometric approach, analyzing 948 relevant publications obtained from the Web of Science Core Collection, SCOPUS, and Science Direct literature databases since 2007. Then, a bibliometric analysis is conducted to obtain the publication's distribution, organization, source, and cooperation networks. Besides, the research hotspots in different periods are identified, and the evolution trend of hot topics is analyzed. Moreover, this paper proposes the possible future research needs in this field. The main hot topics in the field of hydrogen storage and transportation safety research include microstructure, crack, susceptibility, and hydrogen embrittlement and they change over time. In the future, research topics such as hydrogen damage in materials, compatibility of hydrogen in natural gas pipelines, and risk assessment should obtain more attention. ...
Modulating ion-solvent interactions offers a powerful approach to tune the desolvation process, which in turn influences both the capacity and kinetics of electrochemical charge storage. This influence is particularly complex in 2D MXenes due to their surface redox activity and flexible interlayer spacing and thus remains underexplored. In this study, we investigate how tuning the Na+ solvation structure using acetonitrile (ACN) co-solvents affects charge storage mechanism of Ti3C2T x MXene. The addition of ACN enables a new intercalation process at relatively positive potential, which enhances the overall capacitance by ∼30 %. More interestingly, varying the ACN content leads to a transition in the charge storage mechanism of this additional process from non-Faradaic to redox-active. At lower ACN concentrations, strongly solvated Na+ ions intercalate rapidly through a primarily non-Faradaic process, resulting in even better rate retention (72 % at 1 V s-1) than in the pure aqueous electrolyte. Meanwhile, higher ACN content (>50 %) promotes ion desolvation, enabling distinct redox activity (confirmed by in-situ UV–vis) but reduces rate capability. These findings demonstrate a clear correlation between solvation structure and charge storage mechanism in 2D materials, offering a rational strategy to optimize performance via co-solvent design. ...
Journal article (2025) - Benjamin Rui Peng Yip, Chaofan Chen, Yan Jiang, David Ohayon, Guillermo C. Bazan, Xuehang Wang
Despite the development of various pseudocapacitive materials, full-cell pseudocapacitors have yet to surpass the power density of conventional electric double layer capacitors, primarily due to the lack of high-rate positive pseudocapacitive materials. This work reports a solid-state conjugated polyelectrolyte that achieves high-rate charge storage as a positive electrode, facilitated by a co-ion desorption mechanism. The conjugated polyelectrolyte retains 70% of its capacitance at 100 A g−1 with a mass loading of 2.8 mg cm−2 and exhibits a long cycling life of 100,000 cycles in a Swagelok cell configuration. Increasing the electrode thickness fourfold has minimal impact on ion diffusivity and accessibility, yielding a high areal capacitance of 915 mF cm−2. When paired with a high-rate negative pseudocapacitive electrode Ti3C2Tx, the device leverages the redox-active potentials of both materials, achieving a device voltage of 1.5 V and supports operation rates up to 10 V s−1 or 50 A g−1. This configuration enables the pseudocapacitor to deliver an areal power of 160 mW cm−2, while significantly increasing the areal energy (up to 71 μWh cm−2). The high areal performance, combined with the additive-free and water-based fabrication process, makes pseudocapacitors promising for on-chip and wearable energy storage applications. ...
Anode-free aqueous zinc metal batteries (AZMBs) offer significant potential for energy storage due to their low cost and environmental benefits. Ti3C2Tx MXene provides several advantages over traditional metallic current collectors like Cu and Ti, including better Zn plating affinity, lightweight, and flexibility. However, self-freestanding MXene current collectors in AZMBs remain underexplored, likely due to challenges with Zn deposition reversibility. This study investigates the combination of a Ti3C2Tx self-freestanding film with advanced electrolyte engineering, specifically examining the effects of Li-salt and propylene carbonate (PC) as additives on Zn plating reversibility. While using Li+ ions as an additive alone facilitates uniform Zn deposition on bulk metals through the electrostatic shielding effect, the addition of Li-salt negatively impacts Zn plating uniformity on Ti3C2Tx. Meanwhile, using PC additive alone forms an organic SEI layer on Ti3C2Tx and causes Zn agglomeration. The use of both additives together results in a ZnF2-containing hybrid SEI layer with improved interfacial kinetics, promoting more uniform Zn deposition. This approach achieves an average Coulombic efficiency (CE) of 96.8% over 150 cycles (a maximum CE of 97.8%). The study highlights the strategic difference in electrolyte design, emphasizing the need for tailored approaches to optimize Zn deposition on MXenes, contrasting with traditional metallic current collectors. ...
Journal article (2024) - Xiaoyang Guo, Dick van de Kleut, Jia Zhang, Chaofan Chen, Xuehang Wang, Tianye Zheng, Steven Boles
Activated carbon has long been recognized as a promising electrode material for energy storage devices. The extraordinarily high specific area makes it challenging to replace in supercapacitors since electrical double-layer capacitors need such surfaces but also porous networks to enable electrolyte penetration. As a raw material for synthesizing activated carbon, sawdust offers key benefits, such as its renewability, abundance, favorable physical attributes for energy storage, and a more environmentally friendly synthesis process compared to mined alternative sources. In this work, electrochemical characterization is carried out which highlights the critical role of pelletization in enhancing the capacitive performance of sawdust-derived activated carbon, in addition to the implicit handling and logistical benefits. Subsequently, a Li-ion capacitor is assembled with an organic solvent-based electrolyte, sawdust-derived activated carbon serving as the positive electrode, and an Al-based foil negative electrode, potentially combining high energy and power density materials into a hybrid device. Despite commendable electrochemical performance and the use of a sustainable waste-derived positive electrode with a commoditized negative electrode, challenges remain regarding the ability to mitigate the role of surface functional groups that are stabilized by bio-carbon thermal treatments. Nevertheless, this distinctive architecture holds promise as an alternative high-power energy storage technology for a future filled with renewable energy, electric vehicles, and portable electronic devices. ...
Journal article (2024) - Chengzhi Yuan, Chaofan Chen, Baomin Xu, Xuehang Wang, Jun Tang, Zhiwei Yang, Jiaji Cheng, Ji Weng, Shuhui Tan, Renzhong Hou, Tao Cao, Zeguo Tang, Wei Chen
Titanium carbide MXene, Ti3C2Tx, exhibits ultrahigh capacitance in acidic electrolytes at negative potentials yet poor stability at positive potentials, resulting in low-energy densities for Ti3C2Tx-based symmetric supercapacitors. Utilizing “water-in-salt” electrolytes has successfully expanded the stable operation potential window of MXenes. However, this advancement comes at the cost of sacrificing their high capacitance in acidic electrolytes. In this work, we report an acidic “water-in-salt” (AWIS) electrolyte composed of sulfuric acid and saturated lithium halide, which effectively doubled the energy density of the Ti3C2Tx-based symmetric supercapacitor compared to those with bare acidic electrolytes. Specifically, the AWIS electrolyte successfully expanded the voltage window of the symmetric device to 1.1 V. A high specific capacitance of 112.34 F g-1 (at 10 mV s-1) was obtained due to the presence of proton redox. As a result, the symmetric device achieved a high-energy density of 19.1 Wh kg-1 and a high capacitance retention of 96.3% after 10,000 cycles. This work demonstrates the importance of designing stable and redox-active electrolytes for high-energy MXene-based symmetric supercapacitors. ...
Journal article (2024) - Chaofan Chen, Glenn Quek, Simon Fleischmann, Marnix Wagemaker, De en Jiang, Guillermo Carlos Bazan, Xuehang Wang, Hongjun Liu, Lars Bannenberg, Ruipeng Li, Jaehoon Choi, Dingding Ren, Ricardo Javier Vázquez, Bart Boshuizen, Bjørn Ove Fimland
Achieving both high redox activity and rapid ion transport is a critical and pervasive challenge in electrochemical energy storage applications. This challenge is significantly magnified when using large-sized charge carriers, such as the sustainable ammonium ion (NH4+). A self-assembled MXene/n-type conjugated polyelectrolyte (CPE) superlattice-like heterostructure that enables redox-active, fast, and reversible ammonium storage is reported. The superlattice-like structure persists as the CPE:MXene ratio increases, accompanied by a linear increase in the interlayer spacing of MXene flakes and a greater overlap of CPEs. Concurrently, the redox activity per unit of CPE unexpectedly intensifies, a phenomenon that can be explained by the enhanced de-solvation of ammonium due to the increased volume of 3 Å-sized pores, as indicated by molecular dynamic simulations. At the maximum CPE mass loading (MXene:CPE ratio = 2:1), the heterostructure demonstrates the strongest polymeric redox activity with a high ammonium storage capacity of 126.1 C g−1 and a superior rate capability at 10 A g−1. This work unveils an effective strategy for designing tunable superlattice-like heterostructures to enhance redox activity and achieve rapid charge transfer for ions beyond lithium. ...
The growing demand for safe, cost-efficient, high-energy and high-power electrochemical energy storage devices has stimulated the development of aqueous-based supercapacitors with high capacitance, high rate capability, and high voltage. 2D titanium carbide MXene-based electrodes have shown excellent rate capability in various dilute aqueous electrolytes, yet their potential window is usually narrower than 1.2 V. In this study, we show that the potential window of Ti3C2T x MXene can be efficiently widened to 1.5 V in a cost-effective and environmentally benign polyethylene glycol (PEG) containing molecular crowding electrolyte. Additionally, a pair of redox peaks at −0.25 V/−0.05 V vs. Ag (cathodic/anodic) emerged in cyclic voltammetry after the addition of PEG, yielding an additional 25% capacitance. Interestingly, we observed the co-insertion of the molecular crowding agent PEG-400 during the Li+ intercalation process based on in-situ x-ray diffraction analysis. As a result, Ti3C2T x electrodes presented an interlayer space change of 4.7 Å during a complete charge/discharge cycle, which is the largest reversible interlayer space change reported so far for MXene-based electrodes. This work demonstrates the potential of adding molecular crowding agents to improve the performance of MXene electrodes in aqueous electrolytes and to enlarge the change of the interlayer spacing. ...
Book chapter (2023) - Chaofan Chen, Yu Gao, Xuehang Wang
The 2D transition metal carbide and nitride MXenes, especially titanium carbide, are ideal electrode materials for pseudocapacitors due to their metallic conductivity, open interlayer space, and redox-active surface. This article summarizes the electrochemical ion intercalation processes in MXene-based pseudocapacitors with both aqueous and non-aqueous electrolytes. We discuss the impact of ion intercalation on the interfacial characteristics of MXenes, such as interlayer space, surface groups, and interfacial ion-solvent arrangement. Furthermore, we reveal the importance of ion accessibility on the overall pseudocapacitive performance of MXenes and summarize the general strategies to facilitate ion intercalation. ...
Review (2023) - Rui Guo, Chaofan Chen, Lars J. Bannenberg, Hao Wang, Haozhe Liu, Minghao Yu, Zdenek Sofer, Zhibin Lei, Xuehang Wang
Limited Li resources, high cost, and safety risks of using organic electrolytes have stimulated a strong motivation to develop non-Li aqueous batteries. Aqueous Zn-ion storage (ZIS) devices offer low-cost and high-safety solutions. However, their practical applications are at the moment restricted by their short cycle life arising mainly from irreversible electrochemical side reactions and processes at the interfaces. This review sums up the capability of using 2D MXenes to increase the reversibility at the interface, assist the charge transfer process, and thereby improve the performance of ZIS. First, they discuss the ZIS mechanism and irreversibility of typical electrode materials in mild aqueous electrolytes. Then, applications of MXenes in different ZIS components are highlighted, including as electrodes for Zn2+ intercalation, protective layers of Zn anode, hosts for Zn deposition, substrates, and separators. Finally, perspectives are put forward on further optimizing MXenes to improve the ZIS performance. ...