Latest ArticlesMetal-organic frameworks (MOFs) attract broad interests in mercury (Hg) ion adsorption field, while unreasonable distribution of active groups commonly restricts their utilization efficiency. In this work, we constructed a new MOF (TYUST-6) with dense thiol-rich traps in the 1D pore wall. This accessible channel and rational distribution of thiols allow the smooth diffusion of Hg ions and thereby result in a high Langmuir adsorption capacity of 1347.6 mg/g, almost reaching the theoretical maximum (1444.3 mg/g). Adsorption equilibrium needs 10 and 30 min at the initial concentrations of 10 and 100 mg/L, respectively. Common co-existing ions and solution pH show almost negligible interferences on the adsorption, and adsorbent regeneration can be well achieved. Combining experimental characterizations and theoretical calculations, the thiol groups in the pore wall are proved to be the dominant interaction sites. Thus, this work reports a novel high-capacity adsorbent for Hg2+, and proposes a feasible guideline for designing effective adsorbents.
Photodynamic therapy (PDT) presents a promising avenue in cancer treatment. Erlotinib, an FDA-approved anticancer drug targeting epidermal growth factor receptor (EGFR), has shown effectiveness in normalizing tumor vasculature across various tumors, thereby promoting tumor oxygenation and facilitating PDT. In this work, erlotinib was conjugated with a near-infrared (NIR) photosensitizer, benzo[a]phenoselenazinium, yielding three EGFR-targeted PDT agents (NBSe-nC-Er). These newly synthesized photosensitizers demonstrate specificity in binding to EGFR, thereby enhancing their accumulation in cancer cells and tumors, and consequently improving the efficiency of both PDT and chemotherapy. Additionally, the NIR fluorescence emitted by the photosensitizer allows for imaging-guided therapy, offering a non-invasive means of monitoring treatment progress. The distinctive properties of the three-in-one photosensitizer render it an ideal candidate for precise tumor treatment, overcoming the limitations of conventional therapies.
The first total synthesis of (+)-taberdicatine B and (+)-tabernabovine B has been accomplished in 10 steps with 26.9% overall yield and 15 steps with 7.3% overall yield, respectively. The prominent features of this efficient synthetic strategy include the following: (1) (+)-Taberdicatine B and (+)-tabernabovine B were accessed from common advanced intermediates by varying the substituents; (2) A one-pot asymmetric bromocyclization/hydrolysis was explored to assemble HPI skeleton; (3) Dieckmann condensation to form β-keto ester for the assembly of seven-membered ring; (4) An ester reduction/amide semireduction/cyclization sequence was applied to form the cage-like framework.
Two CoⅡ-based complexes, {[Co(dps)2(N3)2]·H2O} (1) and [Co(dps)2(N3)2] (2), show a 1D chain and a 3D network, respectively. The central CoⅡ ions in the complexes have the same coordination environment with the [Co(dps)4(N3)2] unit. Although the differences in crystal parameters are nearly negligible, their magnetic properties are very different. AC susceptibility data show that 1 behaves as a typical field-induced single-ion magnet (SIM) with the out-of-phase (χM'') signals, while 2 shows ac signals of χM'' without peaks even under applied dc filed within our measurement window. Far-IR magneto-spectra (FIRMS) show strong spin-phonon couplings at 0 T in 2, likely making the magnetic relaxation in 2 fast, while the couplings are negligible in 1. Small spin-phonon coupling in 1 likely leads to slower magnetic relaxation, making 1 a SIM. The difference in the properties is due to the structural rigidity of 2 in its 3D network, leading to stronger spin-phonon coupling. Combined high-field EPR (HF-EPR) and FIRMS studies give spin-Hamiltonian parameters, including D = 64.0(9) cm-1, E = 15.7(2) cm-1 for 1 and D = 80.0(2) cm-1, E = 19.0(1) cm-1 for 2.
Current research primarily focuses on emerging organic pollutants, with limited attention to emerging inorganic pollutants (EIPs). However, due to advances in detection technology and the escalating environmental and health challenges posed by pollution, there is a growing interest in treating waters contaminated with EIPs. This paper explores biochar characteristics and modification methods, encompassing physical, chemical, and biological approaches for adsorbing EIPs. It offers a comprehensive review of research advancements in employing biochar for EIPs remediation in water, outlines the adsorption mechanisms of EIPs by biochar, and presents an environmental and economic analysis. It can be concluded that using biochar for the adsorption of EIPs in wastewater exhibits promising potential. Nonetheless, it is noteworthy that certain EIPs like Au(Ⅲ), Rh(Ⅲ), Ir(Ⅲ), Ru(Ⅲ), Os(Ⅲ), Sc(Ⅲ), and Y(Ⅲ), have not been extensively investigated regarding their adsorption onto biochar. This comprehensive review will catalyze further inquiry into the biochar-based adsorption of EIPs, addressing current research deficiencies and advancing the practical implementation of biochar as a potent substrate for EIP removal from wastewater streams.
Defects at the grain boundaries (GBs) of perovskite film highly restrict both the efficiency and stability of perovskite solar cells (PSCs). Herein, organic small molecules of butanedioic acid (BA) and acetylenedicarboxylic acid (AA), containing two carbonyl (C=O) groups and different core-units, were incorporated into perovskite as additives for PSCs application. Thanks to the strong coordination interaction between CO group and under-coordinated Pb2+, the additives can effectively passivate film defects and regulate the perovskite crystallization, yielding high-quality perovskite films with lower defect densities. More importantly, the additives can efficiently regulate the charge transport behaviors in PSCs. Benefiting from the defects passivation and the regulation of charge carrier dynamics, the BA and AA-treaded PSCs show the power conversion efficiencies of 21.52% and 20.50%, which are higher than that of the control device (19.41%). Besides, the optimal devices exhibit a remarkable enhanced long-term stability and moisture tolerance compared to the pristine devices. Furthermore, the transient absorption spectrum reveals the mechanism of enhanced photovoltaic performances, attributing to the improvement of charge transport capability at the perovskite/Spiro-OMeTAD interfaces. This work affords a promising strategy to improve the efficiency and stability of PSCs through regulating the charge-carrier dynamic process in perovskite film.
Rare–earth supramolecular compounds, such as lanthanide organic polyhedrons (LOPs), are of particular interest due to their many possible applications in various fields. Here we report the first syntheses of Ln4(L•+)4–type (Ln, lanthanides; L•+, radical ligand) radical–bridged lanthanide organic tetrahedrons by self–assembly of face–capping triphenylamine (TPA)–cored radical ligand with different lanthanide ions. Remarkable coordination enhanced radical stability has been observed, with half–life times (t1/2) for L1•+, La4(L1•+)4, Eu4(L1•+)4, Gd4(L1•+)4, Tb4(L1•+)4 and Lu4(L1•+)4 estimated to be 53 min, 482 min, 624 min, 1248 min, 822 min and 347 min, respectively. The TPA radical in Ln4(L1•+)4 containing paramagnetic Ln ions (Ln = EuⅢ, GdⅢ and TbⅢ) is observed to be more stable than that in Ln4(L1•+)4 (Ln = LaⅢ and LuⅢ) constructed by diamagnetic Ln ions. This difference in radical stability is possibly due to the magnetic interactions between paramagnetic LnⅢ ions and L1•+ ligands, as confirmed by electron paramagnetic resonance (EPR) in La4(L)4 (L = L1 and L1•+) and Tb4(L)4 (L = L1 and L1•+), and magnetic susceptibility measurements in Tb4(L)4 (L = L1 and L1•+). Our study reveals the coordination of radical ligands with lanthanide ions can improve the radical stability, which is crucial for their applications.
In this work, an effective catalyst of Cu/MnOOH has been successfully constructed for electrochemical nitrate reduction reaction (eNO3RR) for synthesis of ammonia (NH3) under ambient conditions. The substrate of MnOOH plays an important role on the size and electronic structure of Cu nanoparticles, where Cu has the ultrafine size of 2.2 nm and positive shift of its valence states, which in turn causes the increased number of Cu active sites and enhanced intrinsic activity of every active site. As a result, this catalyst realizes an excellent catalytic performance on eNO3RR with the maximal NH3 Faraday efficiency (FE) (96.8%) and the highest yield rate (55.51 mg h−1 cm−2) at a large NH3 partial current density of 700 mA/cm2, which could help to promote the industrialization of NH3 production under ambient conditions.
Carbon dioxide photocatalytic reduction (CO2-PR) is an efficient method for controlling CO2 emissions and generating cleaner energy while mitigating global warming. Tungsten oxides (WxOy) have attracted considerable attention for CO2-PR due to their excellent spectral absorbance. However, comprehensive reviews are lacking on the use of WxOy for CO2-PR. Therefore, this review provides a detailed summary of t research progress made with WxOy-based catalysts in CO2-PR. It also explains the fundamental principles of CO2-PR and evaluates key performance indicators that affect the activity of WxOy-based photocatalysts, including yield, selectivity, stability, and apparent quantum yield. Additionally, this review explores opportunities for synthesizing high-performance WxOy-based photocatalysts and highlights their potential for the green preparation of C1/C2 products through CO2-PR. These innovative strategies aim to address the challenges and pressures associated with energy and environmental issues, particularly by enhancing artificial photosynthesis efficiency.
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