The reformation of catalyst: From a trial-and-error synthesis to rational design

Nano Research, Год журнала: 2023, Номер 17(4), С. 3261 - 3301

Опубликована: Сен. 27, 2023

Язык: Английский

---

Ordered Mesoporous Carbon Grafted MXene Catalytic Heterostructure as Li-Ion Kinetic Pump toward High-Efficient Sulfur/Sulfide Conversions for Li–S Battery

ACS Nano, Год журнала: 2023, Номер 17(2), С. 1653 - 1662

Опубликована: Янв. 6, 2023

Lithium–sulfur (Li–S) batteries exhibit unparalleled theoretical capacity and energy density than conventional lithium ion batteries, but they are hindered by the dissatisfactory "shuttle effect" sluggish conversion kinetics owing to low transport kinetics, resulting in rapid fading. Herein, a catalytic two-dimensional heterostructure composite is prepared evenly grafting mesoporous carbon on MXene nanosheet (denoted as OMC-g-MXene), serving interfacial kinetic accelerators Li–S batteries. In this design, grafted can not only prevent stack of nanosheets with enhanced mechanical property also offer facilitated pump for accelerating diffusion. Meanwhile, exposed defect-rich OMC-g-MXene inhibits polysulfide shuttling chemical interactions between polysulfides thus simultaneously enhances electrochemical efficiency, fully investigated situ/ex situ characterizations. Consequently, cells pumps achieve high cycling (966 mAh g–1 at 0.2 C after 200 cycles), superior rate performance (537 5 C), an ultralow decaying 0.047% per cycle 800 cycles 1 C. Even employed sulfur loading 7.08 mg cm–2 under lean electrolyte, ultrahigh areal 4.5 acquired, demonstrating future practical application.

Язык: Английский

---

Stabilizing Low‐Valence Single Atoms by Constructing Metalloid Tungsten Carbide Supports for Efficient Hydrogen Oxidation and Evolution

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(42)

Опубликована: Сен. 2, 2023

Abstract Designing novel single‐atom catalysts (SACs) supports to modulate the electronic structure is crucial optimize catalytic activity, but rather challenging. Herein, a general strategy proposed utilize metalloid properties of trap and stabilize single‐atoms with low‐valence states. A series supported on surface tungsten carbide (M‐WC x , M=Ru, Ir, Pd) are rationally developed through facile pyrolysis method. Benefiting from WC exhibit weak coordination W C atoms, resulting in formation active centers similar metals. The unique metal‐metal interaction effectively stabilizes single atoms improves orbital energy level distribution sites. As expected, representative Ru‐WC exhibits superior mass activities 7.84 62.52 mg Ru −1 for hydrogen oxidation evolution reactions (HOR/HER), respectively. In‐depth mechanistic analysis demonstrates that an ideal dual‐sites cooperative mechanism achieves suitable adsorption balance H ad OH energetically favorable Volmer step. This work offers new guidance precise construction highly SACs.

Язык: Английский

---

Engineering strategies and active site identification of MXene-based catalysts for electrochemical conversion reactions

Chemical Society Reviews, Год журнала: 2023, Номер 52(9), С. 3215 - 3264

Опубликована: Янв. 1, 2023

This review summarizes engineering strategies to modify MXene-based catalysts and their active site identification for applications in electrochemical conversion reactions.

Язык: Английский

---

Applications of MXene‐Based Single‐Atom Catalysts

Small Structures, Год журнала: 2023, Номер 4(7)

Опубликована: Янв. 27, 2023

Single‐atom catalysts (SACs) consist of isolated metal sites on the support through stable coordination bond, which usually have high catalytic activity and selectivity. With large surface area electron tunability, metallic carbides, nitrides, or carbonic nitrides (MXenes) are suitable carriers for supporting single‐metal atoms. The abundant surface‐functional groups vacancy defects MXenes ideal anchoring Herein, advanced synthesis characterization methods MXene‐based SACs first introduced. Three strategies (adsorption at functional groups, vacancies, terminating group vacancies) appear to be feasible in ensuring non‐aggregation atoms, attributed strong bonding between atoms carrier. applications electrocatalysis (including hydrogen evolution reaction, oxygen reduction carbon dioxide nitrogen reaction), energy storage Li‐ion batteries, metal–air supercapacitors), sensors gas biological sensors) fundamentally reviewed. Finally, own insight current challenges prospects is presented.

Язык: Английский

---

Recent Advances and Perspectives of Lewis Acidic Etching Route: An Emerging Preparation Strategy for MXenes

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Март 15, 2023

Abstract Since the discovery in 2011, MXenes have become rising star field of two-dimensional materials. Benefiting from metallic-level conductivity, large and adjustable gallery spacing, low ion diffusion barrier, rich surface chemistry, superior mechanical strength, exhibit great application prospects energy storage conversion, sensors, optoelectronics, electromagnetic interference shielding biomedicine. Nevertheless, two issues seriously deteriorate further development MXenes. One is high experimental risk common preparation methods such as HF etching, other difficulty obtaining with controllable groups. Recently, Lewis acidic a brand-new strategy for MXenes, has attracted intensive attention due to its safety ability endow uniform terminations. However, comprehensive review etching method not been reported yet. Herein, we first introduce following four aspects: mechanism, terminations regulation, in-situ formed metals delamination multi-layered Further, applications MXene-based hybrids obtained by route sensors microwave absorption are carefully summarized. Finally, some challenges opportunities also presented.

Язык: Английский

---

Recent advances in noble metal MXene-based catalysts for electrocatalysis

Journal of Materials Chemistry A, Год журнала: 2022, Номер 10(28), С. 14674 - 14691

Опубликована: Янв. 1, 2022

In this review, we focus on the recent advances of application noble metal MXene-based catalysts in field electrocatalysis.

Язык: Английский

---

Single-atom CoN4 sites with elongated bonding induced by phosphorus doping for efficient H2O2 electrosynthesis

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 324, С. 122267 - 122267

Опубликована: Дек. 5, 2022

Язык: Английский

---

Recent developments of MXene-based catalysts for hydrogen production by water splitting

Green Chemistry, Год журнала: 2023, Номер 25(5), С. 1749 - 1789

Опубликована: Янв. 1, 2023

In the application of electrolytic water splitting, MXenes can achieve performance optimization by doping, surface functional group regulation, construction defect/vacancy, 3D/porous structure, or compounding with other materials.

Язык: Английский

---

Regulating the Local Electronic Structure of Copper Single Atoms with Unsaturated B,O-Coordination for Selective ¹O₂ Generation

ACS Catalysis, Год журнала: 2023, Номер 13(18), С. 12414 - 12424

Опубликована: Сен. 7, 2023

Generating singlet oxygen (1O2) on single atom catalysts (SACs) in peroxymonosulfate (PMS)-based Fenton-like reactions exhibits great potential for selective degradation of contaminants complex wastewater. Clarifying the structure–activity relationship between electronic structure SACs and 1O2 generation selectivity is crucial precise design efficient catalysts, but it challenging. Herein, Cu with different structures (namely, Cu–O2X, where X = N, S, B, P, O) investigated by density functional theory calculations using adsorption terminal atoms PMS as an activity descriptor. Significantly, affected center which electron-depleted Cu-O2B site a higher atoms. Experimentally, moiety superior catalytic activation, showing nearly 100% ciprofloxacin rate 0.2250 min–1, outperforming those other counterparts. The high attributed to asymmetric accelerating faster electron transfer O–O bond stretching, lowering energy barrier key intermediates toward generation. This work provides broader perspective regulating sites at atomic level catalysts.

Язык: Английский

---