High-Throughput Screening of Synergistic Transition Metal Dual-Atom Catalysts for Efficient Nitrogen Fixation

Nano Letters, Journal Year: 2021, Volume and Issue: 21(4), P. 1871 - 1878

Published: Feb. 15, 2021

Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by discovery of metal–Nx as a promising catalytic center. However, poor activity and low selectivity available SACs are far away from industrial requirement. Through first-principles high-throughput screening, we find that Fe–Fe distributed on graphite carbon nitride (Fe2/g-CN) can manipulate binding strength target species (compromises ability to adsorb N2H NH2), therefore achieving best NRR performance among 23 transition metal (TM) centers. Our results show Fe2/g-CN achieves high theoretical Faradaic efficiency 100% and, impressively, lowest limiting potential −0.13 V. Particularly, multiple-level descriptors shed light origin activity, fast prescreening various candidates. predictions not only accelerate ammonia synthesis but also contribute further elucidate structure–performance correlations.

Language: Английский

---

Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(13)

Published: Feb. 3, 2023

We demonstrate the great feasibility of MBenes as a new class tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As proof concept, FeB2 is first employed model MBene catalyst NO3 RR, showing maximum NH3 -Faradaic efficiency 96.8 % with corresponding yield 25.5 mg h-1 cm-2 at -0.6 V vs. RHE. Mechanistic studies reveal that exceptional RR activity arises from catalysis mechanism, is, B sites activate NO3- form intermediates, while Fe dissociate H2 O and increase *H supply on promote intermediate hydrogenation enhance -to-NH3 conversion.

Language: Английский

---

Electrochemical synthesis of urea on MBenes

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: July 2, 2021

Urea is an important raw material in the chemical industry and widely used as a nitrogen source fertilizers. The current industrial urea synthesis not only requires harsh reaction conditions, but also consumes most of NH3 obtained through artificial synthesis. conversion N2 CO2 into electrochemical reactions under ambient conditions represents novel green method. However, large-scale promotion this method limited by lack suitable electrocatalysts. Here, means density functional theory computations, we systematically study catalytic activity three experimentally available two-dimensional metal borides (MBenes), Mo2B2, Ti2B2, Cr2B2 toward simultaneous electrocatalytic coupling to produce conditions. According our results, these MBenes have superior intrinsic basal for formation, with limiting potentials ranging from -0.49 -0.65 eV, can significantly suppress competitive reduction NH3. In particular, 2D Mo2B2 possess capacity surface oxidation self-corrosion rendering them relatively promising electrocatalysts production. Our work paves way urea.

Language: Английский

---

2D Materials Bridging Experiments and Computations for Electro/Photocatalysis

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 12(4)

Published: Feb. 22, 2021

Abstract The exploration of catalysts for energy conversion lies at the center sustainable development. combination experimental and computational approaches can provide insights into inner laws between catalytic performance structural electronic properties catalysts. Owing to inherent advantages 2D materials over their 3D counterparts, including high specific surface area abundant defects that could sufficient active sites, are promising candidates have attracted wide interest in catalysis. Importantly, most widely computationally investigated models with which relate prediction confirmation conveniently. Recently, more been prepared experiments while accurate methods used disclose performance, explore mechanism an atomic level. In this review, recent advances summarized related development design electro/photocatalysts. main emphasis is put on unique by computations. Computational closer environments introduced particular attention bridge gap addition, challenges computations also discussed

Language: Английский

---

Establishing a Theoretical Landscape for Identifying Basal Plane Active 2D Metal Borides (MBenes) toward Nitrogen Electroreduction

Advanced Functional Materials, Journal Year: 2020, Volume and Issue: 31(6)

Published: Nov. 11, 2020

Abstract To achieve efficient ammonia synthesis via electrochemical nitrogen reduction reaction (NRR), a qualified catalyst should have both high specific activity and large active surface area. However, integrating these two merits into one single material remains big challenge due to the difficulty in balancing multiple intermediates. Here, it is demonstrated that boron‐analogues of MXenes, namely “MBenes”, could cope with region simultaneously toward NRR. Using extensive density functional theory computations taking 16 MBenes as representatives, identified seven (CrB, MoB, WB, Mo 2 B, V 3 B 4 , CrMnB CrFeB ) not only intrinsic basal plane for NRR limiting potentials ranging from −0.22 −0.82 V, but also possess superior capability suppressing competitive hydrogen evolution reaction. Particularly, different MXenes whose oxidation may block sites, once oxidized, can catalyze self‐activating process, reducing O*/OH* H O* under conditions, favoring N electroreduction. As result, exceptional selectivity, area (≈10 19 m −2 ), antioxidation nature render pH‐universal catalysts NH production without introducing any dopants defects.

Language: Английский

---

Immobilizing nZVI particles on MBenes to enhance the removal of U(VI) and Cr(VI) by adsorption-reduction synergistic effect

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 454, P. 140318 - 140318

Published: Nov. 13, 2022

Language: Английский

---

2D MBenes: A Novel Member in the Flatland

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(23)

Published: May 3, 2022

2D MBenes, early transition metal borides, are a very recent derivative of ternary or quaternary boride (MAB) phases and represent new member in the flatland. Although holding great potential toward various applications, mainly theoretical knowledge about their properties is available. Theoretical calculations preliminary experimental attempts demonstrate rich chemistry, excellent reactivity, mechanical strength/stability, electrical conductivity, properties, energy harvesting possibility. Compared to MXenes, MBenes' structure appears be more complex due multiple crystallographic arrangements, polymorphism, structural transformations. This makes synthesis subsequent delamination into single flakes challenging. Overcoming this bottleneck will enable rational control over material-structure-property relationship. Innovations postprocessing approaches allow for design functional systems devices with multipurpose functionalities thus opening promising paradigm conscious high-performance materials.

Language: Английский

---

MBenes: progress, challenges and future

Journal of Materials Chemistry A, Journal Year: 2022, Volume and Issue: 10(30), P. 15865 - 15880

Published: Jan. 1, 2022

The synthesis methods, properties and applications for energy storage electrocatalysis of MBenes were summarized. Furthermore, discussions perspectives on the existing problems, major challenges future development provided.

Language: Английский

---

A Rising 2D Star: Novel MBenes with Excellent Performance in Energy Conversion and Storage

Nano-Micro Letters, Journal Year: 2022, Volume and Issue: 15(1)

Published: Dec. 6, 2022

As a flourishing member of the two-dimensional (2D) nanomaterial family, MXenes have shown great potential in various research areas. In recent years, continued growth interest MXene derivatives, 2D transition metal borides (MBenes), has contributed to emergence this material as latecomer. Due excellent electrical conductivity, mechanical properties and properties, thus MBenes attract more researchers' interest. Extensive experimental theoretical studies that they exciting energy conversion electrochemical storage potential. However, comprehensive systematic review applications not been available so far. For reason, we present summary advances research. We started by summarizing latest fabrication routes MBenes. The focus will then turn their for conversion. Finally, brief challenges opportunities future practical is presented.

Language: Английский

---

Quantum Dots: An Emerging Approach for Cancer Therapy

Frontiers in Materials, Journal Year: 2022, Volume and Issue: 8

Published: Jan. 10, 2022

Nanotechnology is indisputably a scientific technique that offers the prospect of new therapies, and hope, for treatment malignant illnesses. It novel technology approaches diagnosis management diverse diseases. Although discovery Quantum dots (QD) nano-transporters has already led to few positive developments, QD are still at their initial stage, though have yet proven valuable society. The excertion indicates conversion in natural imaging along with photograph established incredible suitability bio-imaging, drug development, targeted gene deliverance, biosensing, photodynamic as well diagnosis. present review aimed confer significance cancer. This aims impart fundamental insight conception its merits, properties, utilization mode action. highlight different designing schemes like hydrothermal, drop-casting, ultrasonic, solvothermal, spin-coating, atomic layer desorption, by layer, polymethylmethacrylate aided-transfer, electrochemical, ion beam sputtering deposition. Moreover, we elaborated on researches related cytotoxic examination reveal QDs harmless. Concisely, summarizes fabrication schemes, current research cancer treatment.

Language: Английский

---