Chemical Engineering Science, Год журнала: 2025, Номер unknown, С. 121573 - 121573
Опубликована: Март 1, 2025
Язык: Английский
Advanced Materials, Год журнала: 2025, Номер unknown
Опубликована: Март 3, 2025
Abstract The upcycling of polyethylene terephthalate (PET)‐derived ethylene glycol (EG) to glycolic acid (GA, a biodegradable polymer monomer) via electrocatalysis not only produces valuable chemicals but also mitigates plastic pollution. However, the current reports for electrooxidation EG‐to‐GA usually operate at reaction potentials >1.0 V vs reversible hydrogen electrode (RHE), much higher than theoretical potential (0.065 RHE), resulting in substantial energy wastage. Herein, body‐centered cubic RhIn intermetallic compounds (IMCs) anchored on carbon support (denoted as RhIn/C) are synthesized, which shows excellent performance with an onset 0.35 RHE, lower values reported literature. catalyst possesses satisfactory GA selectivity (85% 0.65 RHE). Experimental results combined density functional theory calculations demonstrate that IMCs enhance adsorption EG and OH − , facilitating generation reactive oxygen species thereby improving catalytic performance. RhIn/C exhibits electrocatalytic evolution reaction, ensuring it can be used bifunctional two‐electrode system coupled production. This work opens new avenues reducing consumption PET‐derived clean
Язык: Английский
Процитировано
1
Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown
Опубликована: Март 11, 2025
Abstract Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution (HER), conventional approach improve Faradaic efficiency is select a catalyst without HER activity. Nevertheless, such strategy not only limits application of catalysts in NO RR, but also causes insufficient source, thereby sacrificing ammonia yield rate. We believe that should be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co O 4 as model system, we reveal oxygen vacancies on crystal facet can greatly promote dissociation capture intermediate for successfully shifting pathway hydrogenation. Beyond development, construct hybrid reactor achieve an recovery rate 1216.8 g‐N m −2 d −1 nuclear industry wastewater with ultra‐high concentration. This study breaks through limitation which provides significant insight into designing mechanism.
Язык: Английский
Процитировано
1
Angewandte Chemie, Год журнала: 2025, Номер unknown
Опубликована: Март 12, 2025
Abstract Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution (HER), conventional approach improve Faradaic efficiency is select a catalyst without HER activity. Nevertheless, such strategy not only limits application of catalysts in NO RR, but also causes insufficient source, thereby sacrificing ammonia yield rate. We believe that should be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co O 4 as model system, we reveal oxygen vacancies on crystal facet can greatly promote dissociation capture intermediate for successfully shifting pathway hydrogenation. Beyond development, construct hybrid reactor achieve an recovery rate 1216.8 g‐N m −2 d −1 nuclear industry wastewater with ultra‐high concentration. This study breaks through limitation which provides significant insight into designing mechanism.
Язык: Английский
Процитировано
1
Advanced Functional Materials, Год журнала: 2025, Номер unknown
Опубликована: Апрель 13, 2025
Abstract Electrocatalytic nitrate reduction into ammonia (NitRR) over Co‐based catalysts is attractive but still constrained by the competition with H* coupling to produce H 2 . Additionally, fundamental mechanism underlying interfacial engineering associated electronic state transformation for strengthening oriented NitRR remains elusive. Herein, a Co(OH) /Bi 12 O 17 Br heterostructure fabricated using one‐step wet chemistry method, performing remarkable reactivity NH 3 production own formation of electron‐deficiency Co sites induced Bi Unexpectedly, activity increases gradually in initial stage and then keeps at high level, which uncovered as reconstruction 0 Theoretical calculations suggest that situ guides shift d ‐band center toward Fermi thus promoting adsorption conversion intermediates. The synergistic effect hydrolysis dissociation inhibition contributes selectivity NitRR. reconstructed catalyst shows yield rate 7343.3 µg h −1 mg −0.6 V versus RHE nearly 100% Faradaic efficiency −0.4 RHE. This study provides insight
Язык: Английский
Процитировано
1
Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown
Опубликована: Окт. 29, 2024
Abstract The key to fully realizing the potential of high‐entropy alloys (HEAs) lies in balancing their inherent local chemical disordering with long‐range ordering required for electrochemical applications. Herein, we synthesized a distinctive L1 0 ‐(PtIr)(FeMoBi) intermetallics (HEIs) exhibiting nanoscale order and atomic scale short‐range disorder via lattice compensation strategy mitigate entropy reduction tendency. (PtIr)(FeMoBi) catalyst exhibited remarkable activity selectivity glycollic acid (GA) production electrocatalytic waste polymer‐derived ethylene glycol oxidation reaction (EGOR). With mass 5.2 A mg Pt −1 Faradaic efficiency (FE) GA 95 %, it outperformed most previously reported electrocatalysts selective production. lattice‐compensation effect promotes homogeneity Fe actives sites, facilitating co‐adsorption EG OH reducing energy barriers dehydrogenation OH‐combination processes. This approach effectively avoids formation low‐active sites commonly encountered HEA solid solutions, offering promising avenue exploring complex interplay between catalytic HEI structures.
Язык: Английский
Процитировано
7
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(49)
Опубликована: Сен. 4, 2024
Abstract Gallium (Ga) with a low melting point can serve as unique metallic solvent in the synthesis of intermetallic compounds (IMCs). The negative formation enthalpy transition metal‐Ga IMCs endows them high catalytic stability. Meanwhile, their tunable crystal structures offer possibility to tailor configurations active sites meet requirements for specific applications. Herein, we present general method preparing range IMCs, including Co−Ga, Ni−Ga, Pt−Ga, Pd−Ga, and Rh−Ga IMCs. structurally ordered CoGa body‐centered cubic ( bcc ) structure are uniformly dispersed on nitrogen‐doped reduced graphene oxide substrate (O‐CoGa/NG) deliver outstanding nitrate reduction reaction (NO 3 RR) performance, making excellent catalysts construct highly efficient rechargeable Zn‐NO − battery. Operando studies theoretical simulations demonstrate that electron‐rich environments around Co atoms enhance adsorption strength *NO intermediate simultaneously suppress hydrogen, thus improving NO RR activity selectivity.
Язык: Английский
Процитировано
6
Chemical Engineering Journal, Год журнала: 2024, Номер 498, С. 155557 - 155557
Опубликована: Сен. 7, 2024
Язык: Английский
Процитировано
6
ACS Catalysis, Год журнала: 2024, Номер 15(1), С. 156 - 166
Опубликована: Дек. 16, 2024
Electrocatalytic nitrate reduction for ammonia (eNIRR) is an production process that simultaneously removes contaminants from water. However, the lack of activity cathode catalysts used as eNIRR main limiting factor its development. Motivated by this fact, born-doped copper (BDCu) was obtained using ZnO, which easily removed at high temperature, a dispersant, combined with weakly reducing boron clusters (closo-[B12H12]2–) agent and B source during high-temperature pyrolysis. Impressively, BDCu demonstrated Faradaic efficiency 96.58% yield rate 25741.51 μg h–1 mgcat–1 toward −1.8 V (vs saturated calomel electrode). The twice in case undoped B. Evolutionary behavior NO3– to NH3 conversion detected situ Fourier-transform infrared (in FT-IR) electrochemical mass spectrometry DEMS). Experimental density functional theory (DFT) calculations explained activation water enhanced B-doped Cu, adsorption proton *H weakened, made it easy migrate away catalyst required reduction. In addition, electron-deficient provides conditions electron transfer between Cu. Cu led decrease center d-band modulated electronic properties altered transition on surface. Compared well unreduced CuO, lowered energy barrier rate-determining step (*NO → *N), allowing smoother NH3. This study strategy change structure metals B-modification thus improve performance synthesis.
Язык: Английский
Процитировано
6
Advanced Materials, Год журнала: 2024, Номер unknown
Опубликована: Дек. 15, 2024
Ammonia (NH
Язык: Английский
Процитировано
5
Advanced Sustainable Systems, Год журнала: 2025, Номер unknown
Опубликована: Янв. 20, 2025
Abstract Electrocatalytic nitrate reduction (NO 3 RR) offers a promising approach to address pollution by converting harmful nitrates into environment‐benign or valuable products like nitrogen gas (N 2 ) ammonia (NH ). This review explores the mechanisms, challenges, and catalysts involved in NO RR, highlighting role of catalyst selectivity, stability, external reaction conditions. The discussion also covers environmental economic benefits RR for water treatment, alongside potential future directions scaling‐up, system integration, expanding research tackling related nitrogen‐based pollutants as well real world applications.
Язык: Английский
Процитировано
0