Compressive Strain Modulation of Single Iron Sites on Helical Carbon Support Boosts Electrocatalytic Oxygen Reduction DOI
Jia Yang, Zhiyuan Wang, Chunxiang Huang

и другие.

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(42), С. 22722 - 22728

Опубликована: Авг. 17, 2021

Abstract Designing and modulating the local structure of metal sites is key to gain unique selectivity high activity single site catalysts. Herein, we report strain engineering curved atomic iron‐nitrogen boost electrocatalytic activity. First, a helical carbon with abundant high‐curvature surface realized by carbonization polypyrrole that templated from self‐assembled chiral surfactants. The introduces compressive on supported Fe−N 4 sites. Consequently, 1.5 % compressed bonds exhibit downshifted d‐band center than planar Such change can weaken bonding strength between oxygenated intermediates sites, resulting much smaller energy barrier for oxygen reduction. Catalytic tests further demonstrate kinetic current density 7.922 mA cm −2 at 0.9 V vs. RHE obtained in alkaline media which 31 times higher ones. Our findings shed light three‐dimensional boosting catalytic via engineering.

Язык: Английский

Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts DOI
Zhao Chang-xin, Jia‐Ning Liu, Juan Wang

и другие.

Chemical Society Reviews, Год журнала: 2021, Номер 50(13), С. 7745 - 7778

Опубликована: Янв. 1, 2021

Bifunctional oxygen reduction and evolution constitute the core processes for sustainable energy storage. The advances on noble-metal-free bifunctional electrocatalysts are reviewed.

Язык: Английский

Процитировано

534
Design concept for electrocatalysts DOI
Yao Wang, Xiaobo Zheng, Dingsheng Wang

и другие.

Nano Research, Год журнала: 2021, Номер 15(3), С. 1730 - 1752

Опубликована: Сен. 4, 2021

Язык: Английский

Процитировано

488
Non-Bonding Interaction of Neighboring Fe and Ni Single-Atom Pairs on MOF-Derived N-Doped Carbon for Enhanced CO2 Electroreduction DOI
Long Jiao,

Juntong Zhu,

Yan Zhang

и другие.

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(46), С. 19417 - 19424

Опубликована: Ноя. 15, 2021

Single-atom catalysts (SACs), featuring high atom utilization, have captured widespread interests in diverse applications. However, the single-atom sites SACs are generally recognized as independent units and interplay of adjacent is largely overlooked. Herein, by direct pyrolysis MOFs assembled with Fe Ni-doped ZnO nanoparticles, a novel Fe1-Ni1-N-C catalyst, neighboring Ni pairs decorated on nitrogen-doped carbon support, has been precisely constructed. Thanks to synergism pairs, presents significantly boosted performances for electrocatalytic reduction CO2, far surpassing Fe1-N-C Ni1-N-C separate or single atoms. Additionally, also exhibits superior performance excellent CO selectivity durability Zn-CO2 battery. Theoretical simulations reveal that, Fe1-Ni1-N-C, atoms can be highly activated via non-bonding interaction, facilitating formation COOH* intermediate thereby accelerating overall CO2 reduction. This work supplies general strategy construct containing multiple metal species reveals vital importance communitive effect between toward improved catalysis.

Язык: Английский

Процитировано

478
Insights into the activity of single-atom Fe-N-C catalysts for oxygen reduction reaction DOI Creative Commons
Kang Liu, Junwei Fu, Yiyang Lin

и другие.

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Апрель 19, 2022

Single-atom Fe-N-C catalysts has attracted widespread attentions in the oxygen reduction reaction (ORR). However, origin of ORR activity on is still unclear, which hinder further improvement catalysts. Herein, we provide a model to understand Fe-N4 site from spatial structure and energy level frontier orbitals by density functional theory calculations. Taking regulation divacancy defects as examples, demonstrate that hybridization between Fe 3dz2, 3dyz (3dxz) O2 π* activity. We found Fe-O bond length, d-band center gap spin states, magnetic moment *O2 descriptors can accurately predict site. Furthermore, these are mainly distributed two regions with obvious difference, greatly relate height 3d projected orbital Z direction. This work provides new insight into single-atom M-N-C

Язык: Английский

Процитировано

364
Electrocatalysis of Single-Atom Sites: Impacts of Atomic Coordination DOI
Bingzhang Lu, Qiming Liu, Shaowei Chen

и другие.

ACS Catalysis, Год журнала: 2020, Номер 10(14), С. 7584 - 7618

Опубликована: Июнь 11, 2020

Single metal atoms embedded within select supporting matrices have shown great potential in the development of high-efficiency, low-cost electrocatalysts because maximal atom utilization and mass activity. As single are stabilized by coordination bonds with substrate, strong metal–support interactions can be exploited for ready manipulation electrocatalytic activity selectivity toward target reactions. However, most single-atom catalysts (SACs) prepared pyrolysis contain a wide range structures. Resolving atomic configurations moieties represents critical first step establishment an unambiguous correlation between SAC structure In this Review, we summarize recent progress studies electrocatalysts, focus on impacts sites activities series reactions that important various electrochemical energy technologies, such as hydrogen evolution reaction, oxygen reduction nitrogen CO2 so on. The survey entails SACs, from noble metals (e.g., Pt, Pd, Ru, Ir, Au, etc.) to non-noble Fe, Co, Ni, Cu, etc.), supported variety substrate materials pristine doped carbon, metal, oxide, sulfide, etc.). Finally, Review concludes perspective highlighting promises challenges further SACs context chemistry.

Язык: Английский

Процитировано

336
Carbon-based electrocatalysts for sustainable energy applications DOI
Jian Wang, Hui Kong, Jinying Zhang

и другие.

Progress in Materials Science, Год журнала: 2020, Номер 116, С. 100717 - 100717

Опубликована: Июль 18, 2020

Язык: Английский

Процитировано

319
Atomically Dispersed Co2–N6 and Fe–N4 Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media DOI Creative Commons
Zhe Wang, Xiaoyan Jin, Chao Zhu

и другие.

Advanced Materials, Год журнала: 2021, Номер 33(49)

Опубликована: Окт. 8, 2021

Abstract Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based for oxygen reduction reaction (ORR). Regulating the local configuration of atomic is key catalyst performance enhancement. Different from previously reported single‐atom or dual‐atom configurations, a new type ternary‐atom catalyst, which consists atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co 2 –N 6 Fe–N 4 structures) that coanchored on highly graphitized carbon supports developed. This unique ORR outperforms with only in both alkaline acid conditions. Density functional theory calculations clearly unravels synergistic effect sites, can induce higher filling degree Fe–d orbitals favors binding capability *OH intermediates (the rate determining step). may be alternative Pt drive cathodic zinc–air batteries.

Язык: Английский

Процитировано

310
Non-carbon-supported single-atom site catalysts for electrocatalysis DOI
Xiaobo Zheng, Peng Li, Shi Xue Dou

и другие.

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2809 - 2858

Опубликована: Янв. 1, 2021

Non-carbon supported SACs were classified into eight categories based on the nature of their substrates for first time, and corresponding anchoring stabilization mechanisms have been systematically summarized discussed.

Язык: Английский

Процитировано

271
Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis DOI Open Access
Xiaobo Zheng, Beibei Li, Qishun Wang

и другие.

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

Процитировано

264
Ru–Co Pair Sites Catalyst Boosts the Energetics for the Oxygen Evolution Reaction DOI
Xiaobo Zheng, Jiarui Yang,

Zhongfei Xu

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(32)

Опубликована: Май 31, 2022

Abstract Manipulating the coordination environment of active center via anion modulation to reveal tailored activity and selectivity has been widely achieved, especially for carbon‐based single‐atom site catalysts (SACs). However, tuning ligand fields by single‐site metal cation regulation identifying effects on resulting electronic configuration is seldom explored. Herein, we propose a Ru strategy engineer properties constructing Ru/LiCoO 2 SAC with atomically dispersed Ru−Co pair sites. Benefitting from strong coupling between Co sites, catalyst possesses an enhanced electrical conductivity achieves near‐optimal oxygen adsorption energies. Therefore, optimized delivers superior evolution reaction (OER) low overpotential, high mass 1000 A g oxide −1 at small overpotential 335 mV, excellent long‐term stability. It also exhibits rapid kinetics rate capability outstanding durability in zinc–air battery.

Язык: Английский

Процитировано

247