Laser-controlled tandem catalytic sites of CuNi alloys with ampere-level electrocatalytic nitrate-to-ammonia reduction activities for Zn–nitrate batteries

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(7), P. 2991 - 3001

Published: Jan. 1, 2023

Laser-constructed CuNi alloy electrodes with tandem sites of Ni provide H* and Cu for NO 3 − reduction, achieving ampere-level reduction high-performance Zn–NO batteries.

Language: Английский

---

Active site engineering toward atomically dispersed M−N−C catalysts for oxygen reduction reaction

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 495, P. 215400 - 215400

Published: Aug. 21, 2023

Language: Английский

---

Highly Reversible Zn–Air Batteries Enabled by Tuned Valence Electron and Steric Hindrance on Atomic Fe–N₄–C Sites

Nano Letters, Journal Year: 2024, Volume and Issue: 24(15), P. 4672 - 4681

Published: April 8, 2024

The bifunctional oxygen electrocatalyst is the Achilles' heel of achieving robust reversible Zn–air batteries (ZABs). Herein, durable electrocatalysis in alkaline media realized on atomic Fe–N4–C sites reinforced by NixCo3–xO4 (NixCo3–xO4@Fe1/NC). Compared with that pristine Fe1/NC, stability evolution reaction (OER) increased 10 times and reduction (ORR) performance also improved. steric hindrance alters valence electron at sites, resulting a shorter Fe–N bond enhanced sites. corresponding solid-state ZABs exhibit an ultralong lifespan (>460 h 5 mA cm–2) high rate (from 2 to 50 cm–2). Furthermore, structural NixCo3–xO4@Fe1/NC before after OER ORR as well charge–discharge cycling explored. This work develops efficient strategy for improving possibly other processes.

Language: Английский

---

Electronic structure regulation of the Fe-based single-atom catalysts for oxygen electrocatalysis

Nano Energy, Journal Year: 2024, Volume and Issue: 121, P. 109268 - 109268

Published: Jan. 9, 2024

Language: Английский

---

Inhibiting Demetalation of Fe─N─C via Mn Sites for Efficient Oxygen Reduction Reaction in Zinc‐Air Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(32)

Published: May 29, 2024

Demetalation caused by the electrochemical dissolution of metallic Fe atoms is a major challenge for practical application Fe─N─C catalysts. Herein, an efficient single Mn active site constructed to improve strength Fe─N bond, inhibiting demetalation effect Fe─N─C. acts as electron donor inducing more delocalized electrons reduce oxidation state increasing density, thereby enhancing bond and Fe. The oxygen reduction reaction pathway dissociation Fe─Mn dual sites can overcome high energy barriers direct O─O modulate electronic states

Language: Английский

---

Constructing Asymmetrical Coordination Microenvironment with Phosphorus‐Incorporated Nitrogen‐Doped Carbon to Boost Bifunctional Oxygen Electrocatalytic Activity

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(18)

Published: Jan. 17, 2024

Abstract Carbon‐based metal‐free electrocatalysts have been recognized as inexpensive alternatives to afford excellent activity in oxygen reduction/evolution reactions (ORR/OER). Nevertheless, precisely identifying the local active sites and tailoring corresponding electronic properties enhance reaction kinetics remain challenging. Herein, a facile strategy create electrocatalyst comprised of mesoporous nitrogen‐doped carbon matrix with phosphorus incorporation (NPC) is described. The as‐prepared NPC‐950 demonstrates superior ORR under alkaline acidic conditions half‐wave potentials 0.88 0.72 V, respectively, comparable commercial Pt/C (0.85 0.76 V) overwhelmingly other N‐doped catalyst materials. In addition, remarkable promotion OER observed. Notably, zinc–air battery equipped this NCP‐950 exhibits exceptional performance peak power density, specific capacity, long‐term operation durability. Theoretical calculations uncover that NC material results effective charge density redistribution, thus modulating achieve optimum adsorption desorption intermediates. work provides deep understanding heteroatom‐doped materials highlights importance modulation bifunctional electrocatalytic activity.

Language: Английский

---

Lignin‐Metal Supramolecular Framework Strategy of Self‐Healing Carbon‐Coated CoRu Alloy Nanocatalyst for Efficient Overall Water Splitting

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(32)

Published: June 19, 2024

Abstract Common precursors for carbon materials typically include petroleum‐based polymers or MOF materials. However, these often encounter challenges such as metal aggregation, high cost, and metals leaching. In this work, a novel of approach lignin‐metal supramolecular framework complex (MSF@Lignin) is introduced. These complexes are formed through oxidative ammonolysis lignin (OAL) to synthesize nitrogen‐doped carbon‐encapsulated CoRu nanocatalyst (CoRu@OALC) via in situ carbonization. CoRu@OALC exhibited exceptional performance both HER (90 mV) OER (200 at the current density 10 mA cm −2 , with an overall water splitting voltage 1.5 V outstanding stability under density. During pyrolysis process, became encapsulated by lignin‐derived carbon, occurring within temperature range 600–700 °C. catalytic active sites primarily located defects showcasing unique “self‐healing” phenomenon layer. Oxygen‐containing intermediates ( * OH, O, OOH) facilitated reconstruction on layer, while hydrogen‐containing H) contributed reappearance defect‐rich structure.

Language: Английский

---

Photothermal-synergistic peroxymonosulfate activation promoting carbamazepine degradation by Porphyra-derived porous biochar composites: Performance, mechanism, transformation pathway and practical application

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 489, P. 151263 - 151263

Published: April 12, 2024

Language: Английский

---

Surface Engineered Single‐atom Systems for Energy Conversion

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 10, 2024

Abstract Single‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs still early stages of conversion, problems like agglomeration low conversion efficiency hampering their practical applications. Substantial research focus on support modifications, which vital SAC stability due intimate relationship between atoms support. In this review, category supports variety surface engineering strategies employed SA systems summarized, including site (heteroatom doping, vacancy introducing, groups grafting, coordination tunning) structure (size/morphology control, cocatalyst deposition, facet engineering, crystallinity control). Also, merits single‐atom systematically introduced. Highlights comprehensive summary discussions utilization surface‐engineered diversified applications photocatalysis, electrocatalysis, thermocatalysis, devices. At end potential obstacles using field discussed. This review aims guide rational design manipulation target‐specific capitalizing characteristic benefits engineering.

Language: Английский

---

3D Hierarchical MOF-Derived Defect-Rich NiFe Spinel Ferrite as a Highly Efficient Electrocatalyst for Oxygen Redox Reactions in Zinc–Air Batteries

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(9), P. 11537 - 11551

Published: Feb. 16, 2024

The strategy of defect engineering is increasingly recognized for its pivotal role in modulating the electronic structure, thereby significantly improving electrocatalytic performance materials. In this study, we present defect-enriched nickel and iron oxides as highly active cost-effective electrocatalysts, denoted Ni0.6Fe2.4O4@NC, derived from NiFe-based metal–organic frameworks (MOFs) oxygen reduction reactions (ORR) evolution (OER). XANES EXAFS confirm that crystals have a distorted structure metal vacancies. cation defect-rich Ni0.6Fe2.4O4@NC electrocatalyst exhibits exceptional ORR OER activities (ΔE = 0.68 V). Mechanistic pathways electrochemical are studied by DFT calculations. Furthermore, rechargeable zinc–air battery (RZAB) using catalyst demonstrates peak power density 187 mW cm–2 remarkable long-term cycling stability. flexible solid-state ZAB 66 cm–2. proposed structural design allows rational delocalization NiFe spinel ferrite attached to ultrathin N-doped graphitic carbon sheets order enhance site availability facilitate mass electron transport.

Language: Английский

---