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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Triple Amplification Ratiometric Electrochemical Aptasensor for CA125 Based on H-Gr/SH-β-CD@PdPtNFs

Guojuan Zhang,Yujie Han,Zhiguang Liu,Lifang Fan,Yujing Guo

A triple-amplified and ratiometric electrochemical aptasensor for CA125 was designed based on hemin–graphene/SH-β-cyclodextrin@PdPt nanoflower (H-Gr/SH-β-CD@PdPtNF) composites and an exonuclease I (Exo I)-assisted strategy. In the nanocomposite, hemin acts as an internal reference signal owing to the reversible heminox/heminred pair. PdPtNFs can significantly improve the electron transfer rate. SH-β-CD can efficiently enrich quercetin probes through host–guest recognition and increase the second indicator signal. In the presence of CA125, due to the specific binding between the aptamer and CA125, the conformational change of dsDNA (designed by the CA125 aptamer and its complementary DNA) results in the release of quercetin embedded in dsDNA. Subsequently, the free quercetin and DNA fragments are enriched on the H-Gr/SH-β-CD@PdPtNF-modified electrode. Thus, an enhanced oxidation peak from quercetin (IQ) and a reduced peak from hemin (Ihemin) can indicate the same biological identification event. In addition, the recycling amplification of CA125 by Exo I can effectively assist the increase of the quercetin signal. The value of IQ/Ihemin is linear with the concentration of CA125 in the range from 6.0 × 10–4 to 1.0 × 103 ng/mL, and the limit of detection is 1.4 × 10–4 ng/mL. The recovery of CA125 in human blood serum samples was from 99.2 to 104.4%. The proposed sensor is sensitive and reliable, which provides an avenue for the development of triple amplification and ratiometric signal strategies for detecting tumor markers in clinical diagnostics.

CAS / MDL: 18497-13-7 10025-98-6
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Selective Photooxidation of Benzyl Alcohol to Benzaldehyde via H-Abstraction by Bi2.15WO6 under Alkaline Conditions

Wen-Shuang Zhu,Dai Sun,Ling-Li Yu,Shao-Qi Zhi,Yu-Dong Shan,Yi-Fang Lu,Hai-Tao Ren,Song-Hai Wu,Yong Liu,Xu Han

In this study, Bi2.15WO6 with different morphologies was successfully synthesized and used for the selective photooxidation of benzyl alcohol to benzaldehyde in aqueous solutions. High conversion (85%) and selectivity (85%) can be simultaneously achieved under alkaline conditions by adding ethylenediamine to protect the produced benzaldehyde from overoxidation. In the oxidation process, ≡Bi–OO• and ≡Bi–OOH on Bi2.15WO6, instead of OH• and O2•–, are the primary oxidizing species to sequentially abstract two H (H+ + e–) from benzyl alcohol, accompanied by the formation of H2O2. Meanwhile, h+ and OH– also minorly contribute to the selective oxidation of benzyl alcohol via the H-abstraction pathway. This study enriches our understanding of the oxidizing species involved in the selective photooxidation of benzyl alcohol to benzaldehyde.

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Superstable CsxSnBrx+2@CsBr Nanocrystals with Over 1200 h of Half-Value PLQY in Air

Shuang Yang,Yinan Lao,Wenjin Yu,Zhenyu Tang,Haoqing Guo,Ganghong Liu,Bo Qu,Lixin Xiao,Zhijian Chen

Tin-based perovskites comprise one of the preferred nontoxic alternatives to Pb-based perovskites due to their desirable optoelectronic properties. However, there remains a crucial stability problem due to the property of Sn2+ oxidation. In this study, we reported stable tin-based perovskite nanocrystals (NCs) using stannous acetate as the Sn2+ source because of its stronger Sn–O bonding. To prevent the oxidation of Sn2+, a thin layer of CsBr coverage was formed in situ; tin-based perovskite NCs, CsxSnBrx+2@CsBr (1 < x < 4), show a high photoluminescence quantum yield (PLQY) of 78.2% and high stability. The measured lifetime of PLQY decrease to half of the initial value is ∼1287 h under ambient conditions and ∼2200 h under a nitrogen atmosphere, respectively. Furthermore, the as-fabricated light-emitting diodes based on CsxSnBrx+2@CsBr NCs as the emitting layer exhibit a maximum luminescence of 16 cd/m2 and an external quantum efficiency of 0.035% with peaks at 451 and 615 nm, corresponding to the emissions of CsBr and CsxSnBrx+2, respectively. This work provided a new way to obtain stable Sn-based perovskite NCs and exhibited their potential for application in white light-emitting diodes (LEDs).

CAS / MDL: 3396-11-0
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RADIATION RESEARCH · 2023 ·Vol. 200 ·期 3 ·242-255 · IF 3.4

Advances in Polymeric Neutron Shielding: The Role of Benzoxazine-h-BN Nanocomposites in Nuclear Protection

Abdous Slimane,Derradji Mehdi,Mekhalif Zineb,Khiari Karim,Mehelli Oussama,Cherif Younes Bourenane

Given their substantial neutron capture cross-section, extreme hardness, and high chemical and thermal stability, boron-based materials are widely used as building blocks to protect against highly ionizing radiations such as gamma rays and neutrons. Indeed, uncontrolled nuclear radiation exposure can be highly hazardous to radiation workers and the public. In this sense, this work presents an extensive study and experimental evaluation of the nuclear shielding features of hexagonal-boron nitride (h-BN) based nanocomposite, where bisphenol-A based polybenzoxazine (BA-PBz) was used as matrix. The neutron shielding studies were carried out at the nuclear research reactor of Algeria NUR. The surface treatment of h-BN nanoparticles was confirmed by FTIR and XPS techniques. The curing behavior and the degradation phenomena of the nanocomposites were evaluated by DSC-TGA analyses. The distribution of h-BN nanoparticles within the polymer matrix was assessed by TEM and SEM. The results showed that the developed boron nitride-based nanocomposite exhibits intriguing shielding performances and good thermal stability. The DSC-TGA tests exhibit high degradation temperature that reach 279°C. The highest performances were obtained at an h-BN concentration of 7 wt%, where the macroscopic cross was found to be (Σ = 3.844 cm –1 ) with a screening ratio of (S = 96.12%), equivalent to a mean free path (λ) of 0.138 cm.

CAS / MDL: 80-05-7 30525-89-4
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FUEL · 2022 · IF 8.035

Selectively converting fructose to furfural over H-beta zeolite: Elucidating the roles of framework aluminum

Yueqing Wang,Hongxing Wang,Junbo Zhang,Hongyan Zheng,Long Huang,Yulei Zhu

Selectively converting fructose into furfural by H-beta catalyst is a very interesting catalytic process. However, it is a challenging task to clearly elucidate the roles of framework Al for selective scission of C C and C O bond. Herein, selective elimination of framework Al atoms is realized. Several detailed investigations showed that the framework Al species located in different sites play important role in furfural formation. The framework Al atoms of pristine H-beta mainly occupied at T1, T2, T5, T6 and T7 sites. These Al species at pore mouth can be removed by citric acid, while the treatment of nitric acid mainly eliminated the framework Al atoms from T2 and T7 sites. As for oxalic acid, the Al atoms occupied at T2, T5, T6 and T7 was primarily leached. Upon citric acid and nitric acid treatment afforded the similar yield of furfural, indicating that the formation of furfural could not be governed by these Al species at pore mouth, T2 and T7 sites. However, in the case of oxalic acid treatment, complete removal of the Al species on T2, T5, T6 and T7 sites decreased the yield of furfural. Thus, it is reasonably inferred that these Al atoms populated at T1 sites and intersecting channels is more encouraging for the splitting of C C bond, while the Al species occupied at T5, T6 sites and the larger straight channels is probably more favorable to scission of C O bond.

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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2022 · IF 6.364

Densification mechanism and corrosion resistance of h-BN/ZrO2 ceramics prepared by spark plasma sintering

Mao chen,Fan Zhang,Hailong Wang,Gang Shao,Bingbing Fan,Rui Zhang,Hongxia Li,Yongqiang Chen

The dense h-BN/ZrO 2 (30 wt%) composites without additives were rapidly fabricated by spark plasma sintering . The relative density, apparent porosity, fracture toughness, flexural strength , phase composition and microstructure of h-BN/ZrO 2 composites were systematically investigated. Besides, the corrosion resistance of h-BN/ZrO 2 composites in molten steel was also studied in detail. Especially, the h-BN/ZrO 2 composites were sintered at 1800 °C exhibiting a relative density of 96.6% and the flexural strength of ≈ 157 MPa. The corrosion of h-BN/ZrO 2 composites was mainly due to the oxidative decomposition of BN, and the corrosion process was clarified by a parabolic law. The excellent corrosion resistance of the h-BN/ZrO 2 composites was attributed to ZrO 2 residual layer formed at the interface. The corrosion thickness of h-BN/ZrO 2 composites was only ∼116 µm even using the longest corrosion time (80 min). The composites could be a promising candidate material applied to fabricated thin strip continuous casting side sealing plates.

CAS / MDL: 10043-11-5 1314-23-4
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Self-Adaptive Dirhodium Complexes in a Metal–Organic Framework for Synthesis of N–H Aziridines

Zhenzhong Li,Huating Jiang,Jinxiu Liu,Tiantian Ning,Nam T. S. Phan,Fang Zhang

Conformational dynamics of active sites in enzymes enable great control over the catalytic process. Herein, we constructed a metal–organic framework with conformationally dynamic active sites (Rh2-ZIF-8). The active sites in Rh2-ZIF-8 were composed of the imidazolate-bridged bimetallic center with a catalytic dirhodium moiety and structural zinc site. Even though the coordination sphere of the dirhodium species was saturated with two circularly arranged esp groups and two axial 2-MeIm ligands, it could still effectively catalyze the direct synthesis of N–H aziridines from olefins with high activity. We found that such a self-adaptive catalytic process was based on the dynamic breakage and reformation of the rhodium–zinc imidazolate bridges. Interestingly, the in situ generated dirhodium site with a unique Rh2(esp)2(2-MeIm)1 configuration was able to exhibit obviously enhanced selectivity compared to homogeneous catalyst Rh2(esp)2. Furthermore, the surrounding zinc imidazolate groups could effectively protect the dirhodium moieties from harsh environments, and this ultimately endowed it with high stability.

CAS / MDL: 693-98-1 10196-18-6
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PROGRESS IN ORGANIC COATINGS · 2022 · IF 6.206

Fluoro-substituted polyaniline deeply incorporation with inert h-BN for interface improvement in anti-corrosion

Cheng Li,Xiao Wang,Meng Zhang,Yue Sun,Yexiang Cui,Yanji Zhu,Huaiyuan Wang

Inert inorganic anti-corrosion fillers enjoy the advantages of stable performance, but most of them face the problems of poor compatibility and disability. Therefore, strategies about addressing the above problems need to be developed. Herein, based on interface enhancement strategy, one typical inert inorganic filler h-BN was armed with fluoro-substituted polyaniline (PFAN). To this end, diazotization reaction was utilized to introduce aniline group to h-BN, and emulsion polymerization was employed to grow the micro-size copolymer of aniline and 2-fluoroaniline. Benefitting from the above interface enhancement attempt, the compatibility of h-BN with resin was enhanced, which was explained by the chemical armed PFAN participated in the curing process of epoxy. Moreover, the disability of h-BN was also improved owed to this interface armor. Therefore, combining the fully developed barrier properties of h-BN with passivate ability of PFAN, the coating containing a small addition amount (0.9 wt%) of the composite fillers to epoxy coatings significantly improved their long-term corrosion resistance , which was confirmed by the EIS result that its low frequency impedance value was maintained above 10 10 and was about 10 3 times larger than that of pure EP coating after being immersed in 3.5 wt% NaCl solution for 120 days.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Enhanced catalytic behavior of h-BN supported CuNi bimetallic catalysts in hydrolytic dehydrogenation of NH3BH3

Kexin Liu,Shilong Yang,Yi Chen,Wenlei Zhang,Pu Liu,Xiucheng Zheng

The hydrolysis of ammonia borane (NH 3 BH 3 , AB) is an efficient strategy for high-purify hydrogen evolution . However, it is indispensable to develop a suitable catalyst because this reaction is kinetically infeasible at room temperature . In this work, we prepared a series of nano hexagonal boron nitride (h-BN) supported CuNi bimetallic catalysts through a facile adsorption-chemical reduction procedure. The effects of various molar ratios of Cu to Ni and CuNi loadings on AB hydrolysis were investigated in details. Benefitting from the proper porous structure , the interesting alloy effect of Cu and Ni, as well as the synergistic effect between h-BN and CuNi, 20 wt% Cu 0.5 Ni 0.5 /h-BN displays the highest catalytic activity among the as-prepared catalysts. Apart from satisfactory durability, the corresponding hydrogen generation rate, turnover frequency at 303 K in base solution and apparent activation energy are 2437.0 mL g −1 min −1 , 6.33 min −1 and 23.02 kJ mol −1 , respectively, which are very outstanding compared with many previous results. Our work not only provides a proper non-precious metal catalyst for hydrogen generation from the hydrolysis of chemical hydrogen storage materials but also offers a facile strategy for synthesizing metallic functional materials .

CAS / MDL: 10043-11-5
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2022 · IF 6.76

Bi@H-TiO2/B-C3N4 heterostructure for enhanced photocatalytic hydrogen generation activity under visible light

Junfeng Yang,Yuyang Wu,Yanhui Dong,Hao Cui,Chenyang Shi,Hang Sun,Shengyan Yin

Herein, a ternary Bi@H-TiO 2 /B-C 3 N 4 type II heterostructure is successfully designed and prepared via metal Bi as cocatalyst for photocatalytic H 2 generation. As expected, under λ > 300 nm light, the highest photocatalytic hydrogen production rate (HPR) of Bi@H-TiO 2 /B-C 3 N 4 is up to 223.08 μmol g −1  h −1 . Excitingly, under visible light (λ > 400 nm), the highest HPR of Bi@H-TiO 2 /B-C 3 N 4 is increased to 18.84 μmol g −1  h −1 , which is about 67.3 times, 37.7 times and 6.8 times as high as that of H-TiO 2 , B-C 3 N 4 and H-TiO 2 /B-C 3 N 4 under the same conditions, respectively. Moreover, the electrochemical impedance spectroscopy and transient photocurrent tests manifest that the interface resistance of Bi@H-TiO 2 /B-C 3 N 4 composite decreases and the photocurrent density increases after loading metal Bi. These results indicate that loading metal Bi as cocatalyst (providing more electron trapping sites) is beneficial to improve photocatalytic activity in the type II heterostructure composite. And the electron transfer directions (B-C 3 N 4  → H-TiO 2  → Bi or B-C 3 N 4  → Bi) are proved by ultraviolet photoelectron spectroscopy test. Therefore, the Bi@H-TiO 2 /B-C 3 N 4 photocatalyst with strong visible light absorption is expected to be a promising candidate in photocatalytic fields under visible light.

CAS / MDL: 10035-06-0
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INDUSTRIAL CROPS AND PRODUCTS · 2022 · IF 6.449

Deconstruction of H-bonding and crystallite in directly prepared cellulose nanofibrils after autohydrolysis of eucalyptus

Yachong Zhu,Yehong Chen,Chaojun Wu,Dongmei Yu,Qijun Ding,Ronggang Li

In this study, cellulose nanofibrils (CNFs) were directly prepared after autohydrolysis of eucalyptus raw materials. The effect of different autohydrolysis times on the hydrogen bond structure, micro-structure and properties of CNFs were analyzed by FTIR peak fitting, two-dimensional infrared, TGA, TEM and X-ray diffractometer. The results showed that the autohydrolysis treatments could obviously lead to the sequence of hydrogen bond changes in CNFs as follows: v (weak hydrogen bond) > v (free hydroxyl) > v (O(3)H.O(5)) > v (O(2)H.O(6)) >  v (O(6)H.O(3′)), and further impact in crystallite size of CNFs. With the increase of the autohydrolysis strength, the crystallite size of CNFs on the 1 1 ¯ 0 crystal plane could be reduced by up to 26%, but the crystallite size on the 110 crystal plane and the 200 crystal plane increased by 24.5% and 22.6%, respectively. These microstructure changes finally increased the crystallinity index of CNFs, and then resulted in their high thermal stability.

CAS / MDL: 7758-02-3
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ADVANCED SYNTHESIS & CATALYSIS · 2022 ·Vol. 364 ·期 8 ·1450-1459 · IF 5.981

Development of an NAD(H)-Driven Biocatalytic System for Asymmetric Synthesis of Chiral Amino Acids

Feng Cheng,Jia-Min Zhang,Zhen-Tao Jiang,Xiao-Hu Wu,Ya-Ping Xue,Yu-Guo Zheng

Chiral amino acids are extensively applied in the pharmaceutical, food, cosmetic, and agricultural industries. As a representative example, l -phosphinothricin ( l -PPT, a chiral non-natural amino acid) is a broad-spectrum herbicide. An NAD(H)-driven biocatalytic system for the asymmetric synthesis of chiral amino acids (focused on l -PPT) with high efficiency and low cost is highly desired. The key for the development of such biocatalytic system is to obtain an NADH-dependent biocatalyst with high catalytic performance toward l -PPT pro-ketone PPO. Herein, an engineered glutamate dehydrogenase from Lysinibacillus composti ( Lc GluDH) with desired activity was obtained by gene mining and protein engineering. In silico analyses suggested that the volume of substrate-binding pocket was substantially enlarged from 330.5 Å 3 to 409.6 Å 3 . The stability of Lc GluDH was increased ( T m value increased from 47.3 °C to 65.3 °C) by introducing positively charged amino acids or aromatic amino acids at position 375. The desired biocatalytic system was constructed by coupling the engineered Lc GluDH and an NAD + -dependent FDH. Through this biocatalytic system, the batch production of l -PPT exhibited high space-time yield (207.3 g ⋅ L −1 ⋅ day −1 ) with strict stereoselectivity ( ee of l -PPT>99%). Furthermore, eight other chiral amino acids were synthesised by the developed NAD(H)-driven biocatalytic system with high ee values.

CAS / MDL: 53-84-9 51276-47-2
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