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Electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species

Publication . Zhang, Zheng; Li, Danyang; Tu, Yunchuan; Deng, Jiao; Bi, Huiting; Yao, Yongchao; Wang, Yan; Li, Tingshuai; Luo, Yongsong; Sun, Shengjun; Zheng, Dongdong; Carabineiro, Sónia A. C.; Chen, Zhou; Zhu, Junjiang; Sun, Xuping; LAQV@REQUIMTE; DQ - Departamento de Química

The electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality and reduce environmental pollution, but also establishes a route to synthesize valuable chemicals, such as urea, amide, and amine. This innovative approach expands the application range and product categories beyond simple carbonaceous species in electrocatalytic CO2 reduction, which is becoming a rapidly advancing field. This review summarizes the research progress in electrocatalytic urea synthesis, using N2, NO2−, and NO3− as nitrogenous species, and explores emerging trends in the electrosynthesis of amide and amine from CO2 and nitrogen species. Additionally, the future opportunities in this field are highlighted, including electrosynthesis of amino acids and other compounds containing C–N bonds, anodic C–N coupling reactions beyond water oxidation, and the catalytic mechanism of corresponding reactions. This critical review also captures the insights aimed at accelerating the development of electrochemical C–N coupling reactions, confirming the superiority of this electrochemical method over the traditional techniques.

2024-04Recensão

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Multifunctional MgAl LDH/Zn-MOF S-scheme heterojunction

Publication . Maseeh, Ihsan; Anwar, Farheen; Aroob, Sadia; Javed, Tariq; Bibi, Ismat; Almasoudi, Afaf; Raheel, Ahmad; Javid, Muhammad Arshad; Carabineiro, Sónia A. C.; Taj, Muhammad Babar; LAQV@REQUIMTE; DQ - Departamento de Química; RSC - Royal Society of Chemistry

Metal-organic frameworks (MOFs) and layered double hydroxides (LDHs) are undoubtedly promising and valuable materials for developing advanced catalysts to achieve efficient hydrogen evolution. The unique structures, environmentally friendly nature, and high redox activities of these materials make them ideal for catalytic applications. In this study, a delicately constructed S-scheme heterojunction photocatalyst, denoted as MgAl LDH/Zn-MOF, was designed and synthesized through the in situ nucleation of Zn-MOF nanostructure on MgAl LDH nanosheets, based on their excellent electronic properties and opposite surface potential. The MgAl LDH/Zn-MOF photocatalyst exhibited enhanced photocatalytic hydrogen evolution activity (129 mmol g−1) compared to Zn-MOF and MgAl LDH alone. This was mainly due to the formation of the MgAl LDH/Zn-MOF S-scheme heterojunction, which effectively accelerated the recombination of several electrons (from the conduction band of Zn-MOF) and holes (from the valence band of MgAl LDH), thus preventing the recombination of other electrons (from the conduction band of MgAl LDH) and holes (from the valence band of Zn-MOF), which is a critical requirement for efficient hydrogen evolution. Further, the MgAl LDH/Zn-MOF has a high potential for methyl red removal (97% following the intraparticle diffusion model with a maximum R2 value of 0.996). The CO2 adsorption isotherms of the MgAl LDH/Zn-MOF revealed a gravimetric CO2 uptake capacity of 129.7 mg g−1 (at 298 K and 40 bar) and stable cyclic adsorption performance. These findings demonstrate the potential of MOFs and LDHs for developing advanced catalysts for efficient hydrogen evolution and highlight the importance of heterojunction design.

2024-06-17Artigo científico

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Exploring the catalytic and anticancer activity of gold(I) complexes bearing 1,3,5-triaza-7-phosphaadamantane (PTA) and related ligands

Publication . Conceição, Nuno Reis; Mahmoud, Abdallah G.; Dietl, Martin C.; Caligiuri, Isabella; Rizzolio, Flavio; Carabineiro, Sónia A. C.; Rudolph, Matthias; Silva, M. Fátima C. Guedes da; Pombeiro, Armando J. L.; Hashmi, A. Stephen K.; Scattolin, Thomas; LAQV@REQUIMTE; DQ - Departamento de Química; DCEA - Departamento de Ciências e Engenharia do Ambiente; RSC - Royal Society of Chemistry

A series of water-soluble gold(i) complexes bearing phosphine ligands, [AuCl(L)] {where L = 1,3,5-triaza-7-phosphaadamantane, PTA (1); 3,7-diacetyl-1,3,7-triaza-5-phosphabicyclo[3.3.1]nonane, DAPTA (2); or 1,3,7-triaza-5-phosphabicyclo[3.3.1]nonane-3,7-diylbisphenylmethanone, DBPTA (3)} and [AuCl(L)]X {where L is either PTA-CH2-C6H4-p-COOH and X = Br (4) or PTA-CH2-C6H3-p-OH-m-CHO and X = Cl (5)}, were synthesized under mild conditions and characterized with multinuclear (1H, 13C and 31P) nuclear magnetic resonance (NMR) spectroscopy, attenuated total reflection - Fourier transform infrared (ATR-FTIR) spectroscopy, matrix-assisted laser desorption/ionization - mass spectrometry (MALDI-MS) and elemental analysis. The catalytic activity of the complexes was evaluated in the peroxidative oxidation of cyclohexane to cyclohexanol and cyclohexanone. Homogeneous reactions were conducted in aqueous media, while heterogeneous reactions were performed after immobilizing the complexes on porous carbon supports, including activated carbon (AC), carbon nanotubes (CNT) and their oxidized derivatives (AC-ox, AC-ox-Na, CNT-ox and CNT-ox-Na). The results demonstrated a better catalytic performance, in terms of yields and selectivity, under heterogeneous conditions depending on the nature of the carbon support. Finally, complexes 1-5 showed remarkable cytotoxicity against a selection of ovarian, lung and colon cancer cell lines, with IC50 values comparable to (or even better than) those of cisplatin. Interestingly, the most promising complexes exhibited good to excellent cytotoxicity against cancer cells while demonstrating substantial inactivity against normal ones.

2025-04-04Artigo científico

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Synergistic Effect of NiAl-Layered Double Hydroxide and Cu-MOF for the Enhanced Photocatalytic Degradation of Methyl Orange and Antibacterial Properties

Publication . Batool, Iqra; Aroob, Sadia; Anwar, Farheen; Taj, Muhammad Babar; Baamer, Doaa F.; Almasoudi, Afaf; Ali, Omar Makram; Aldahiri, Reema H.; Alsulami, Fatimah Mohammad H.; Khan, Muhammad Imran; Nawaz, Aamir; Maseeh, Ihsan; Nazir, Muhammad Khalid; Carabineiro, Sónia A.C.; Shanableh, Abdallah; Fernandez-Garcia, Javier; LAQV@REQUIMTE; DQ - Departamento de Química; Faculdade de Ciências e Tecnologia (FCT); MDPI - Multidisciplinary Digital Publishing Institute

This study synthesized NiAl-layered double hydroxide (LDH)/Cu-MOF photocatalyst using a simple impregnation method involving NiAl-LDH and Cu-MOF. The successful synthesis was confirmed through Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), zeta potential measurements, thermogravimetric analysis (TGA), ultraviolet diffuse reflectance spectroscopy (UV-DRS), N2 adsorption at −196 °C, and electrochemical impedance spectroscopy (EIS). Photocatalysts based on NiAl-LDH, Cu-MOF, and NiAl-LDH/Cu-MOF were used to remove methyl orange (MO) dye from contaminated water. The impact of various factors, including pH, dye concentration, and photocatalyst amount, on MO degradation efficiency was assessed. FTIR analysis was conducted both before and after dye degradation. The optimal degradation conditions were a photocatalyst dose of 25 mg and a pH of 3. Kinetic studies indicated that the degradation of MO dye onto NiAl-LDH/Cu-MOF followed a pseudo-first-order and an L–H or Langmuir–Hinshelwood model. The value of R2 = 0.94 confirms the validity of pseudo-first-order and Langmuir–Hinshelwood (L–H) kinetic models for the photocatalytic degradation of MO dye. This study highlights the importance of developing novel photocatalysts with improved degradation efficiency to protect the water environment. Antibacterial activity was also performed with antibacterial sensibility testing by disk diffusion to determine minimal inhibitory and bactericidal concentrations. In short, NiAl-LDH/Cu-MOF can be helpful for various biomedical and industrial applications.

2024-10Artigo científico

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Catalysis by Metal-Oxide Nanostructures

Publication . Carabineiro, Sónia Alexandra Correia; LAQV@REQUIMTE; DQ - Departamento de Química; MDPI AG

2024-02-24Editorial de revista

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