Polyester Upcycling to Glycine via Tandem Thermochemical–Electrochemical Catalysis DOI
Yingxin Ma, Wenxuan Chen,

Wenfang Yuan

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 12, 2024

Abstract Deconstruction of polyethylene terephthalate (PET) plastics into commodity chemicals such as glycine presents a promising route for waste valorization. However, directly upcycling PET via thermocatalysis typically requires harsh conditions (e.g., high H 2 pressure and elevated temperature) while suffering from limited selectivity carbon footprint. Herein, cascade thermochemical–electrochemical catalysis is developed to exploit end‐of‐life with yield, without the use hydrogen gas in entire process. first degraded oxalic acid thermochemical oxidative depolymerization using an active robust HY‐zeolite‐supported Au catalyst under low O (0.3 MPa), then valorize intermediate two‐step electroreduction over earth‐abundant TiO catalyst. The proposed approach resilient impurities realistic streams, enables continuous conversion various goods overall yield 75%. Techno‐economic analysis life cycle assessment demonstrate that cost‐effective low‐carbon upcycling. This hybrid technology paves way leverage mitigating plastic pollution producing high‐value chemicals.

Language: Английский

Subnanometric Nickel Phosphide Heteroclusters with Highly Active Niδ+–Pδ− Pairs for Nitrate Reduction toward Ammonia DOI
Qi Hu, Chunyan Shang, Xinbao Chen

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The development of efficient electrocatalysts for the neutral nitrate reduction reaction (NO3–RR) toward ammonia (NH3) is essential to address environmental issues caused by NO3– but remains considerably challenging owing sluggish kinetics NO3–RR in media. Herein, we report subnanometric heteroclusters with strongly coupled nickel–phosphorus (Ni–P) dual-active sites as boost NO3–RR. Experimental and theoretical results reveal that feature Ni–P promotes electron transfer from Ni P, generating Niδ+–Pδ− active pairs, which Niδ+ species are highly Pδ− tunes interfacial water hydrogen bonding network promote dissociation step accelerate proton during Consequently, NO3–RR, exhibit a large NH3 yield rate 0.61 mmol h–1 cm–2 at −0.8 V versus reversible electrode, 2.8- 3.3-fold larger than those on nanoparticles clusters, respectively, generated exists NH4+ electrolytes. This study offers an approach boosting electrocatalytic reactions multiple intermediates designing sites.

Language: Английский

Citations

2
Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc‐Air Batteries DOI
Siqi Ji,

Yimin Mou,

Hongxue Liu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(44)

Published: Sept. 16, 2024

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity stability is a crucial, yet challenging step to achieving conversion. Here, an approach address this issue: synthesis atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over porous, defect‐containing nitrogen‐doped carbon support, described. Through incorporation phosphorus atom into the second coordination sphere iron, durability boundaries catalyst pushed unprecedented level alkaline environments, such as those found zinc‐air battery. The rationale delicately incorporate P heteroatoms defects close central metal sites (FeN 4 ‐OH) order break local symmetry electronic distribution. This enables suitable binding strength oxygenated intermediates. In situ characterizations theoretical studies demonstrate that these synergetic interactions responsible for stability. These intrinsic advantages /NCP enable potential gap mere 0.65 V power density 263.8 mW cm −2 when incorporated findings underscore importance design principles access high‐performance green

Language: Английский

Citations

14
Modulating Hydrogen Adsorption by Unconventional p–d Orbital Hybridization over Porous High‐entropy Alloy Metallene for Efficient Electrosynthesis of Nylon‐6 Precursor DOI

Youwei Sheng,

Jiangwei Xie,

Ruidong Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(44)

Published: July 12, 2024

Renewable electricity driven electrosynthesis of cyclohexanone oxime (C

Language: Английский

Citations

12
Boosting Amino Acid Synthesis with WOx Sub‐Nanoclusters DOI Open Access

Guanzheng Wu,

Zengying Ma,

Tobias Heil

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 12, 2025

Abstract The conversion of nitrate‐rich wastewater and biomass‐derived blocks into high‐value products using renewably generated electricity is a promising approach to modulate the artificial carbon nitrogen cycle. Here, new synthetic strategy WO x sub‐nanoclusters reported supported on materials as novel efficient electrocatalysts for nitrate reduction its coupling with α‐keto acids. In acidic solutions, NH 3 ‐NH 2 OH selectivity can also optimized by adjusting potential, total FE exceeding 80% over wide potential range. After introducing acids, /D‐CB electrode achieves remarkable activity toward C ‐C 6 amino For glycine alanine, impressive FEs 49.34% 38.22% based transitional metal oxides be obtained, surpassing those nanoclusters larger size. situ analysis mechanistic studies reveal critical role in reducing energy barriers key steps alanine synthesis. This work opens up insights rational design cluster catalysts promote electrochemical acid

Language: Английский

Citations

1
Research Progress of Coordination Materials for Electrocatalytic Nitrogen Oxides Species Conversion into High-Value Chemicals DOI
Xianlong Liu, Peisen Liao, Weifang Liao

et al.

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100146 - 100146

Published: Feb. 1, 2025

Language: Английский

Citations

1
Cu–Bi Bimetallic Catalysts Derived from Metal–Organic Framework Arrays on Copper Foam for Efficient Glycine Electrosynthesis DOI
Peisen Liao,

Binning Zeng,

Suisheng Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 30, 2024

Abstract Glycine as one of the most abundant amino acids in human proteins, with extensive applications both life and industry, is conventionally synthesized through complex procedures or toxic feedstocks. In this study, we present a facile benign electrochemical pathway for synthesis glycine reductive coupling glyoxylic acid nitrate over copper‐bismuth bimetal catalyst derived from metal–organic framework (MOF) array on copper foam (Cu/Bi−C@CF). Remarkably, Cu/Bi−C@CF achieves fantastic selectivity 89 %, corresponding high Faraday efficiency 65.9 %. From control experiments, introduction Bi caused binding energy Cu shift to lower state, which leads towards formation key intermediate hydroxylamine rather than ammonia product, facilitating oxime providing additional sites subsequent hydrogenation reaction way glycine. Moreover, derivation MOF arrays ensures effective dispersion enhances stability Cu/Bi−C@CF. This innovative approach not only presents sustainable pathways production value‐added organonitrogen compounds utilizing readily available carbon nitrogen sources, but also provides novel insights into design multistage structural catalysts sequential reactions.

Language: Английский

Citations

8
Enhanced nitrite electroreduction to ammonia via interfacial dual-site adsorption DOI

Xiaokang Chen,

Shengliang Zhai,

Yi Tan

et al.

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 96, P. 328 - 335

Published: May 13, 2024

Language: Английский

Citations

7
Oriented Synthesis of Glycine from CO2, N2, and H2O via a Cascade Process DOI Open Access
Xiangdong Kong, Chunxiao Liu,

Zifan Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(50)

Published: Aug. 28, 2024

Abstract Air contains carbon, hydrogen, oxygen, and nitrogen elements that are essential for the constitution of amino acids. Converting air into acids, powered with renewable electricity, provides a green sustainable alternative to petrochemical‐based methods produce waste pollution. Here, taking glycine as an example, we demonstrated complete production chain electrorefining acids directly from CO 2 , N H O. Such prospective Scheme was composed three modules, linked by spontaneous C−N bond formation process. The high‐purity bridging intermediates, separated stepwise synthesis, boosted both carbon selectivity 91.7 % 98.7 %. Under optimum condition, obtained partial current density 160.8 mA cm −2 . solid product acquired separation efficiency 98.4 This work unveils method abiotic creation components.

Language: Английский

Citations

4
Advances and perspectives on photochemical/electrochemical synthesis of nitrogen, sulfur, and phosphorus heteroatom containing compounds from biomass-based feedstocks DOI

Hanjing Tian,

Anping Wang, Pan Hu

et al.

Industrial Crops and Products, Journal Year: 2024, Volume and Issue: 222, P. 119738 - 119738

Published: Sept. 27, 2024

Language: Английский

Citations

4
Theoretical study on the synthesis of glycine via electrocatalytic reduction over tandem catalysts based on two-dimensional carbon-rich conjugated metalloporphyrin frameworks DOI

Xuan Niu,

Ling Guo

New Journal of Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

FeY-Cr(Zr)-BPor COF catalysts not only maintain the advantages of bimetallic but also utilize role B atoms to fully activate NO and CO 2 , thereby exhibiting good catalytic activity with a very low limiting potential (−0.20 V).

Language: Английский

Citations

0