Rare-Earth Single-Atom La–N Charge-Transfer Bridge on Carbon Nitride for Highly Efficient and Selective Photocatalytic CO₂ Reduction

ACS Nano, Journal Year: 2020, Volume and Issue: 14(11), P. 15841 - 15852

Published: Nov. 3, 2020

Photocatalytic CO2 conversion into valuable solar fuels is highly appealing, but lack of directional charge-transfer channel and insufficient active sites resulted in limited reduction efficiency selectivity for most photocatalytic systems. Herein, we designed fabricated rare-earth La single-atoms on carbon nitride with La-N bridge as the center reaction. The formation was certified by spherical aberration-corrected HAADF-STEM, STEM-EELS, EXAFS, theoretical calculations. electronic structure enables a high CO-yielding rate 92 μmol·g-1·h-1 CO 80.3%, which superior to g-C3N4-based reductions. production remained nearly constant under light irradiation five cycles 20 h, indicating its stability. closely combined experimental DFT calculations clearly elucidated that variety states induced 4f 5d orbitals single atom p-d orbital hybridization atoms enabled channel. charge bridges are found function key activation, rapid COOH* formation, desorption. present work would provide mechanistic understanding utilization photocatalysis energy conversion.

Language: Английский

---

Graphene aerogel-based NiAl-LDH/g-C3N4 with ultratight sheet-sheet heterojunction for excellent visible-light photocatalytic activity of CO2 reduction

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 306, P. 121065 - 121065

Published: Jan. 21, 2022

Language: Английский

---

Layered double hydroxide‐based photocatalytic materials toward renewable solar fuels production

InfoMat, Journal Year: 2021, Volume and Issue: 3(7), P. 719 - 738

Published: May 7, 2021

Abstract Photocatalysis is an ideal and promising green technology to drive numerous chemical reactions for valued chemicals production under very mild conditions, thereby providing solutions global energy environment issues related burning fossil fuels. Over the past decade, layered double hydroxides (LDHs), as members in two‐dimensional materials family, have attracted much attention due their many advantages photocatalysis, such facile synthesis, low cost powerful tunability of composition. In this review, we provide a synthetic overview recent research advances LDH‐based photocatalysts, with main discussion design strategies improve photocatalytic performance, including component control, defect engineering, hybridization, topological transformation. Structure‐performance correlations tailor‐made material synthesis are elaborated discuss how realize high‐performance photocatalysts three important (i.e., water splitting, CO 2 conversion, N reduction) generate desirable solar Further, remaining challenges future perspectives summed up, aiming inspire brand new pushing forward development photocatalysis. image

Language: Английский

---

Phosphorus Tailors thed‐Band Center of Copper Atomic Sites for Efficient CO₂Photoreduction under Visible‐Light Irradiation

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(38)

Published: July 8, 2022

Photoreduction of CO2 into solar fuels has received great interest, but suffers from low catalytic efficiency and poor selectivity. Herein, two single-Cu-atom catalysts with unique Cu configurations in phosphorus-doped carbon nitride (PCN), namely, Cu1 N3 @PCN P3 were fabricated via selective phosphidation, tested visible light-driven reduction by H2 O without sacrificial agents. was exclusively active for CO production a rate 49.8 μmolCO gcat-1 h-1 , outperforming most polymeric (C3 N4 ) based catalysts, while preferably yielded . Experimental theoretical analysis suggested that doping P C3 replacing corner C atom upshifted the d-band center close to Fermi level, which boosted adsorption activation on making efficiently convert CO. In contrast, much lower 3d electron energy exhibited negligible adsorption, thereby preferring formation photocatalytic splitting.

Language: Английский

---

Integrating Dual-Metal Sites into Covalent Organic Frameworks for Enhanced Photocatalytic CO₂ Reduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(7), P. 4316 - 4329

Published: March 15, 2023

Photocatalytic CO2 reduction holds great promise for synchronously addressing carbon neutrality and producing fuels, although enhancing the photocatalyst activity tuning product selectivity remain enormous challenges. Herein, we synthesized four crystalline porous benzothiadiazole-based covalent organic frameworks (COFs) with different carbonyl groups reported a dual metalation strategy to fabricate Co Ni dual-metal sites anchored on COFs by interaction between metal thiadiazole high-performance photoreduction. Among as-synthesized metalated Co/Ni sites, CoNi–COF-3 achieved an impressive CO generation rate of 2567 μmol g–1 h–1 92.2%, which were significantly higher than those single sites. Experimental theoretical results revealed that superior photocatalytic performance was attributed synergic effect fully β-ketoenamine-tautomerized COF-3 configuration not only facilitated photogenerated charge carrier dynamics but also reduced energy barriers *COOH formation promoted adsorption desorption. This work provides valuable insights into future design improved COF photocatalysts conversion.

Language: Английский

---

Spatial distribution of ZnIn2S4 nanosheets on g-C3N4 microtubes promotes photocatalytic CO2 reduction

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 418, P. 129476 - 129476

Published: March 24, 2021

Language: Английский

---

In-situ construction of BiOBr/Bi2WO6 S-scheme heterojunction nanoflowers for highly efficient CO2 photoreduction: Regulation of morphology and surface oxygen vacancy

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 452, P. 139493 - 139493

Published: Sept. 30, 2022

Language: Английский

---

Research progress on photocatalytic reduction of CO₂ based on LDH materials

Nanoscale, Journal Year: 2022, Volume and Issue: 14(9), P. 3367 - 3386

Published: Jan. 1, 2022

Converting CO2 to renewable fuels or valuable carbon compounds is an effective way solve the global warming and energy crisis. Compared with other conversion methods, photocatalytic reduction of more energy-saving, environmentally friendly, has a broader application prospect. Layered double hydroxide (LDH) attracted widespread attention as two-dimensional material, composed metal layers, interlayer anions water molecules. This review briefly introduces basic theory photocatalysis mechanism reduction. The composition properties LDH are introduced. research progress on in field elaborated from six aspects: directly catalyst, precursor for by modification, intercalation, supporting materials construction heterojunction. Finally, development prospects put forward. could provide reference efficient reasonable photocatalysts based LDH.

Language: Английский

---

Emerging Strategies for CO₂ Photoreduction to CH₄: From Experimental to Data‐Driven Design

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(20)

Published: March 29, 2022

Abstract The solar‐energy‐driven photoreduction of CO 2 has recently emerged as a promising approach to directly transform into valuable energy sources under mild conditions. As clean‐burning fuel and drop‐in replacement for natural gas, CH 4 is an ideal product photoreduction, but the development highly active selective semiconductor‐based photocatalysts this important transformation remains challenging. Hence, significant efforts have been made in search active, selective, stable, sustainable photocatalysts. In review, recent applications cutting‐edge experimental computational materials design strategies toward discovery novel catalysts photocatalytic conversion are systematically summarized. First, insights effective catalyst engineering strategies, including heterojunctions, defect engineering, cocatalysts, surface modification, facet single atoms, presented. Then, data‐driven photocatalyst spanning density functional theory (DFT) simulations, high‐throughput screening, machine learning (ML) presented through step‐by‐step introduction. combination DFT, ML, experiments emphasized powerful solution accelerating reduction . Last, challenges perspectives concerning interplay between rational industrialization large‐scale technologies described.

Language: Английский

---

Internal electric field engineering step-scheme–based heterojunction using lead-free Cs3Bi2Br9 perovskite–modified In4SnS8 for selective photocatalytic CO2 reduction to CO

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 313, P. 121426 - 121426

Published: April 21, 2022

Language: Английский

---