Latest ArticlesMIL-88A(Fe)@sponge (MS) was synthesized by a dip-coating method, which displayed efficient photocatalytic Cr(Ⅵ) reduction efficiency under both low power LED UV light and real solar light irradiation. It was observed that MS (0.2 g/L) could remove 100% Cr(Ⅵ) (10 mg/L) by adding 0.4 mmol/L tartaric acid (TA) without adjusting pH (pH 5.05) within 6.0 min and 3.0 min under UV light and real solar light irradiation, respectively. Besides, the photo-induced e− and radicals (O2•− and CO2•−) were found to play the momentous roles in the MS/TA/UVL/Cr(Ⅵ) system by the scavenger experiments and electron spin resonance (ESR) tests. MS was also filled into a fixed-bed reactor to test the possibility of long-term Cr(Ⅵ) reduction operation in TA/UVL system. As expected, the results revealed that MS could still maintain 100% activity up to 60 h. These results demonstrated that MIL-88A(Fe) might be the potentially efficient catalyst for large-scale wastewater treatment in the near future.
Decarbonylation of aldehydes is a basic organic transformation, which has been developed for more than six-decade. However, as comparing to well-studied aromatic aldehydes, fewer examples for catalytic decarbonylation of aliphatic aldehydes were reported, mainly on simple or special substrates. For α-bulky or highly functionalized ones, stoichiometric Rh(Ⅰ) were usually required for decent yields. Herein, we present a rare example of Ir(Ⅰ)-catalyzed direct decarbonylation of α-quaternary aldehydes with broad substrate scope and good functional group compatibility via judicious selection of ligand. The α-chirality is memorized in this decarbonylation process. In addition, we report a broad-spectrum decarbonylation of α-secondary and α-tertiary aldehydes containing multifunctional groups with an improved Rh(Ⅰ)/DPPP recipe. Finally, we realized selective decarbonylation of α-tertiary aldehydes in the presence of α-quaternary one via the reactivity differences.
Hydrogen production from water electrolysis using renewable electricity is a highly promising route to solve the energy crisis of human society. The tetragonal 3d-transition metal selenide with metallic feature has been discovered to efficiently catalyze the hydrogen evolution electrocatalysis; however, its performance is still unsatisfactory and further improvement is necessary. Herein, the hydrogen evolution reaction of the functional tetragonal 3d-transition metal selenide with the heteroatom-dopant as well as cationic vacancy is fully investigated by means of density functional theory calculations. Our results identify 53 promising candidates endowed with good activity due to the absolute free energy of hydrogen adsorption |∆GH| ≤ 0.30 eV wherein 15 candidates with |∆GH| ≤ 0.09 eV possess compelling performance in comparison with the benchmark Pt material. Interestingly, the functional CuSe systems account for 29 out of 53 candidates, being high attractive for experimental synthesis. According to the analysis of electronic structure, the enhanced performance stems from the upshift of the sp orbitals, which benefits for the improved affinity toward hydrogen capture. This work provides new direction and guidance for the design of novel electrocatalysts.
Copper is one of the most efficient catalysts widely investigated in electrochemical CO2 reduction, however, the further development of copper-based catalysts is constrained by severe stability problems. In this work, we developed a method for the synthesis of highly ordered CuAu intermetallic nanoalloys (o-CuAu) under mild conditions (< 250 ℃), which can convert carbon dioxide to carbon monoxide with high selectivity and can operate stably for 160 h without current decay. The improved stability is believed to be due to the increased mixing enthalpy and stronger atomic interactions between Cu and Au atoms in the intermetallic nanoalloy. In addition, XPS results, Tafel slope and in situ IR spectroscopy demonstrate that high valence gold atoms on o-CuAu surface promote the reduction of CO2. In contrast, the disordered CuAu nanoalloy (d-CuAu) underwent atomic rearrangement to form a Cu-rich structure on the surface, leading to reduced stability. These findings may provide insight into the rational design of stable CO2RR electrocatalysts through proper structural engineering.
The binding interactions between 4-aminopyridine (4-AP) and a series of cucurbit[n]urils (Q[5], Q[6], TMeQ[6], Q[7], Q[8]) have been studied using 1H NMR spectroscopy, UV–vis absorption spectroscopy, isothermal titration calorimetry (ITC) and X-ray crystallography. The data indicates that the Q[5]@4-AP complex exhibits exo binding, which is not observed in the other four host-guest complexes. Furthermore, X-ray crystallography clearly reveals how the Q[n]s bind with 4-AP to form complexes, for example Q[5] forms an outer-surface complex, whilst Q[6], TMeQ[6] and Q[7] formed 1:1 host and guest type complexes, and Q[8] formed a stable 1:2 ternary complex due to its large cavity, which can accommodate two 4-AP molecules.
A chronic liver disease usually results in iron accumulation, and an excess of iron will further aggravate liver injury, forming a vicious circle. Likewise, it also plays a significant role in other organs when it comes to iron metabolism. A long time passes between the time it takes to break through to MRI-based iron diagnosis and its ability to distinguish the types of iron accumulation accurately and quickly. This work highlighted a new type of iron accumulation treatment solution integrated with diagnosis and treatment. A chelating method for ICG and Leci that can assist PAI and MRI to achieve better diagnostic and therapeutic effects. This work revealed biomaterial engineering techniques are being adapted to address clinical medical problems through cutting-edge research.
Heteroatom-doped porous carbon materials are very attractive for lithium ion batteries (LIBs) owing to their high specific surface areas, open pore structures, and abundant active sites. However, heteroatom-doped porous carbon with very high surface area and large pore volume are highly desirable but still remain a big challenge. Herein, we reported a sulfur-doped mesoporous carbon (CMK-5-S) with nanotubes array structure, ultrahigh specific surface area (1390 m2/g), large pore volume (1.8 cm3/g), bimodal pore size distribution (2.9 and 4.6 nm), and high sulfur content (2.5 at%). The CMK-5-S used as an anode material for LIBs displays high specific capacity, excellent rate capability and highly cycling stability. The initial reversible specific capacity at 0.1 A/g is as high as 1580 mAh/g and simultaneously up to 701 mAh/g at 1 A/g even after 500 cycles. Further analysis reveals that the excellent electrochemical storage performances is attributed to its unique structures as well as the expanded lattice by sulfur-doping.
Non-centrosymmetric chalcogenides are attracting considerable attention as highly promising infrared nonlinear optical (IR-NLO) candidates, but it is challenging to simultaneously achieve sufficient second-harmonic-generation coefficient (deff > 0.5 × AgGaS2) and large energy gap (Eg > 3.5 eV). In this work, a novel ternary chalcogenide, Cs5Ga9S16 with an ultra-wide Eg of 4.05 eV, has been successfully obtained. This sulfide belongs to the monoclinic space group Pn (No. 7) with a novel 3D anionic [Ga9S16]5– framework that is formed by super-polyhedral [Ga9S23] units through corner-sharing S atoms. Such a unique crystal structure displays desirable characteristics which indicate a promising IR-NLO candidate: favourable phase-matching feature, sufficient deff (0.7 × AgGaS2), ultrahigh laser-induced damage threshold (31.6 × AgGaS2) and broad transparent region (0.27−14.96 µm). In addition, systematic theoretical studies and structural analysis suggest that the desirable IR-NLO performances can be attributed to the super-polyhedral building blocks. This finding may provide useful insight into the understanding and designing other high-performance IR-NLO candidates with super-polyhedral-built structures.
78Li2S-22P2S5 are sulfide electrolytes with high lithium-ion conductivity and wide electrochemical windows in the Li2S-P2S5 system, making them attractive solid electrolytes for ASSLBs. However, the role and potential of 78Li2S-22P2S5 solid electrolytes over a wide temperature range are still not fully understood. Therefore, we constructed solid-state batteries with NCM622 as the positive electrode and 78Li2S-22P2S5 glass-ceramics as the electrolyte to investigate in depth the differences in battery performance over a wide temperature range and their intrinsic mechanisms. The in-situ impedance and relaxation time distribution (DRT) demonstrated the electrochemical stability of the electrolyte over a wide temperature range, while the in-situ stacking pressure observed a large volume change during cycling at 60 ℃, leading to local solid-solid contact failure and poor cycling stability. This study provides insight into the advantages and problems of 78Li2S-22P2S5 in the wide temperature range as well as a basis for the construction of ASSLBs with high energy density and long cycle life.
The development of excellent catalyst to achieve photocatalytic syngas production from CO2 and H2O is a prospective and sustainable strategy to alleviate environment and energy crisis. In this study, a unique Janus PdZn-Co catalyst is prepared by annealed the Pd/IRMOF-3(Co, Zn) precursor. Due to the strong interaction, the electron transfers from PdZn terminal to Co terminal in the Janus structure. The electron-received Co terminal facilitates Co sites coordinate with the electrophilic C atom of CO2 and the electron-donated PdZn center is easier to coordinate with nucleophilic O atoms of H2O or CO bonds. The charge redistribution enhances the absorption of CO2 and H2O, which promotes H2 evolution and CO production. In addition, the carbon shell effectively suppresses the metal core agglomeration and facilitates the electron transmission from photosensitizer to metallic active sites. Meanwhile, the ratio of CO/H2 can be regulated (~3:1 to 2:1) by adjusting the proportion of Co and PdZn. The Janus structure and graphite carbon synergistically play a profound impact on improving the photocatalytic performance. The optimized PdZn-Co catalyst exhibits a superior photocatalytic CO production rate (20.03 µmol/h) and the H2 generation rate (9.90 µmol/h) with a ratio of CO/H2 = 2.02.
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