MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2

Zhao, Di; Chen, Zheng; Yang, Wenjuan; Liu, Shoujie; Zhang, Xun; Yu, Yi; Cheong, Weng‐Chon; Zheng, Lirong; Ren, Fuqiang; Ying, Guobing; Cao, Xing; Wang, Dingsheng; Peng, Qing; Wang, Guoxiu; Chen, Chen

doi:10.1021/jacs.8b13579

Cited by 500 publications

(424 citation statements)

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“…It exhibits high durability and outstanding hydrogen evolution reaction activity. Later on, a similar material based on Ti 3 C 2 O 2 MXene has been prepared and used as an electrocatalyst for CO 2 RR, in which Pt atom was confined in the Ti vacancy …”

Section: Introductionmentioning

confidence: 99%

“…Inspired by these experimental progresses, we explored the potential application of single atom embedded MXene nanosheets in electrocatalytic NRR. Because Mo plays an essential role in biological nitrogen fixation system, and a series of Mo‐containing materials have been studied as the promising NRR catalysts, here we chose Mo 2 TiC 2 O 2 as the substrate to construct SACs.…”

Section: Introductionmentioning

confidence: 99%

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Theoretical Screening of Single Transition Metal Atoms Embedded in MXene Defects as Superior Electrocatalyst of Nitrogen Reduction Reaction

et al. 2019

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The MXene‐supported single transition metal systems have been reported as promising electrocatalysts for hydrogen evolution reaction (HER) and carbon dioxide reduction reaction. Herein, the potential performance of MXene‐based catalysts was explored on nitrogen reduction reaction (NRR). Density functional theory computations are carried out to screen a series of transition metal atoms confined in a vacancy of MXene nanosheet (Mo2TiC2O2). The results reveal that the Zr, Mo, Hf, Ta, W, Re, and Os supported on defective Mo2TiC2O2 layer can significantly promote the NRR process. Among them, Zr‐doped single atom catalyst (Mo2TiC2O2‐ZrSA) possesses the lowest barrier (0.15 eV) of the potential‐determining step, as well as high selectivity over HER competition. To the best of knowledge, 0.15 eV is the lowest barrier of potential‐determining step that has been reported for NRR so far. Besides, the formation energy of Mo2TiC2O2‐ZrSA is much more negative than that of the synthesized Mo2TiC2O2‐PtSA catalyst, suggesting that the experimental preparation of Mo2TiC2O2‐ZrSA is feasible. This work thus predicts an efficient electrocatalyst for the reduction of N2 to NH3 at ambient conditions.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Theoretical Screening of Single Transition Metal Atoms Embedded in MXene Defects as Superior Electrocatalyst of Nitrogen Reduction Reaction

et al. 2019

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“…The active sites could be intuitively discerned from the bright spots in the HAADF‐STEM images due to the different Z value of dispersed metal atoms in comparison with the atoms of the supports . For instance, Ti 3− x C 2 T y nanosheets supported with single Ru atoms (Ru 1 /Ti 3− x C 2 T y ), Ru 1 /Ti 3− x C 2 T y were synthesized by uniformly absorbing [RuCl 6 ] 2− on the surface of Ti 3− x C 2 T y nanosheets, and slowlybeing reduced and stabilized by reductive Ti vacancies . HAADF‐STEM and element mapping images presented that Ru atoms homogeneously distributed on the Ti 3− x C 2 T y nanoflakes and no individual Ru nanoparticles were observed ( Figure a).…”

Section: Characterization Techniques Of Sacs For Biomedical Applicationsmentioning

confidence: 99%

“…a,b) HAADF−STEM images and corresponding element mapping images of Ru 1 /Ti 3‐x C 2 T y (a) and Ir 1 /Ti 3‐x C 2 T y (b). a,b) Reproduced with permission . Copyright 2019, American Chemical Society.…”

Section: Characterization Techniques Of Sacs For Biomedical Applicationsmentioning

confidence: 99%

Single‐Atom Catalysts in Catalytic Biomedicine

2020

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The intrinsic deficiencies of nanoparticle‐initiated catalysis for biomedical applications promote the fast development of alternative versatile theranostic modalities. The catalytic performance and selectivity are the critical issues that are challenging to be augmented and optimized in biological conditions. Single‐atom catalysts (SACs) featuring atomically dispersed single metal atoms have emerged as one of the most explored catalysts in biomedicine recently due to their preeminent catalytic activity and superior selectivity distinct from their nanosized counterparts. Herein, an overview of the pivotal significance of SACs and some underlying critical issues that need to be addressed is provided, with a specific focus on their versatile biomedical applications. Their fabrication strategies, surface engineering, and structural characterizations are discussed briefly. In particular, the catalytic performance of SACs in triggering some representative catalytic reactions for providing the fundamentals of biomedical use is discussed. A sequence of representative paradigms is summarized on the successful construction of SACs for varied biomedical applications (e.g., cancer treatment, wound disinfection, biosensing, and oxidative‐stress cytoprotection) with an emphasis on uncovering the intrinsic catalytic mechanisms and understanding the underlying structure–performance relationships. Finally, opportunities and challenges faced in the future development of SACs‐triggered catalysis for biomedical use are discussed and outlooked.

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“…[ 38 ] Chen's group reported a facile synthesis route to achieve single Pt atoms on Ti 3− x C 2 T y nanosheets (Pt 1 /Ti 3− x C 2 T y ) with a Pt loading of ≈0.2 wt%. [ 39 ] Under mild conditions, Ti vacancies were prepared by hydrochloric acid etching of parent Ti 3 AlC 2 . During the etching process, some TiAl bonds were broken, followed by the removal of Al layers and adjacent Ti atoms ( Figure a).…”

Section: Synthesis Of Single‐atom Catalytic Materialsmentioning

confidence: 99%

Single‐Atom Catalytic Materials for Advanced Battery Systems

2020

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power and energy densities are the imperative units for these cutting-edge energy harvesting and storage. [3] The state-ofthe-art commercial batteries are prepared with graphite anodes and lithium transition-metal oxide cathodes that reversibly intercalate lithium (Li) ions with moderate stability and energy densities. [4] The intrinsic physicochemical properties and ion insertion mechanisms of conventional materials limits the energy capacity of devices, which will not be quantified for unprecedented demand of modern electronics. [5] Other than the insertiontype electrode materials, there exist some conversion-type electrode materials with higher energy storage capability and faster electrochemical conversion dynamics, including transition-metal dichalcogenide (TMD) and silicon materials. [6] TMD materials demonstrate strong chemical interaction and high catalytic effect with active species in batteries, which is critical to suppress shuttle effects and promote conversion kinetics. [7] But lithiation of TMD materials inevitably gives rise to phase transformation and causes severe damage for the structural integrity of electrodes. [8] Silicon materials emerge as promising conversion-type substitute in recent years due to the high theoretical capacity of 4200 mAh g −1 , but silicon materials exit severe volume expansion effect in conversion processes, which will lead to rapid capacity degradation within several cycles. [9] These two typical conversion-type materials are both semiconductor materials with poor conductivity and unsatisfactory structural stability under electrochemical conditions. Construction of composition architectures with carbon materials is a common strategy to address these drawbacks for purpose of increasing conductivity and maintaining structural integrity. [10] Even if some synthetic methods have been deliberately considered and rationally designed, their attractive theoretical capacities have not fully expressed with long-term cycling performances. Thus, novel battery chemistries other than traditional insertion and conversion-type electrode materials need to be developed to address these issues.With the ever-increasing development of material science and engineering, lots of alternative materials with high energy capacities and stabilities have stood out as the electrode materials from the competition with conventional counterparts. For instance, sulfur material-based batteries gives high theoretical Advanced battery systems with high energy density have attracted enormous research enthusiasm with potential for portable electronics, electrical vehicles, and grid-scale systems. To enhance the performance of conversiontype batteries, various catalytic materials are developed, including metals and transition-metal dichalcogenides (TMDs). Metals are highly conductive with catalytic effects, but bulk structures with low surface area result in low atom utilization, and high chemical reactivity induces unfavorable dendrite effects. TMDs present chemical adsorption with active species and ...

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MXene (Ti₃C₂) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO₂

Cited by 500 publications

References 39 publications

Theoretical Screening of Single Transition Metal Atoms Embedded in MXene Defects as Superior Electrocatalyst of Nitrogen Reduction Reaction

Theoretical Screening of Single Transition Metal Atoms Embedded in MXene Defects as Superior Electrocatalyst of Nitrogen Reduction Reaction

Single‐Atom Catalysts in Catalytic Biomedicine

Single‐Atom Catalytic Materials for Advanced Battery Systems

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