CHEMISTRY OF MATERIALS
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2019
·
IF 10.159
Bingquan Jia,Wei Zhao,Du Sun,Linggang Fan,Heliang Yao,Ping Lu,FangFang Xu,Fuqiang Huang
Solution-mediated sequential ion exchange has emerged as a powerful yet simple technique to transform nanoparticulates into a complex architecture. However, the state-of-the-art demonstration of such fine-tailored nanostructures greatly relied on cation exchange reaction because it remains to be a great challenge to apply anion exchange without interfering the original morphology and crystallinity of the target particles. Herein, metal cyanamides with a looser cation sublattice enabled by the quasi-linear [NCN]2– anion units are discovered to be ideal parent compounds to accomplish robust anion exchange reactions. The complete conversion from metal cyanamide nanoparticles to metal chalcogenide nanoparticles (CdNCN to CdS, CdNCN to CdSe, and MnNCN to MnS) is successfully realized by low-temperature reaction in colloidal solution. The nanoparticles retain both the morphology and crystallinity throughout the entire exchange process. In-depth study reveals that the structural similarity in cation packing facilitates the exchange process, and such behavior is independent of the material composition. The quasi-linear structure of the three-atom [NCN]2– anion results in anisotropic lattice spaciousness, which helps bypass the diffusion rate discrepancy and lattice framework collapse commonly encountered in compounds consisting of single-atom anions. This work sheds light on extending the ion exchange reactions as a synthetic toolbox to a much broader library in nanoparticle synthesis.
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ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Guangli He,Yunhe Lai,Yanzhen Guo,Hang Yin,Binbin Chang,Man Liu,Shouren Zhang,Baocheng Yang,Jianfang Wang
Designing plasmonic photocatalysts with spatially controlled catalytic sites is an effective strategy to boost the sunlight-driven chemical transformation efficiency through plasmonic enhancement. Herein, we describe a facile method for the synthesis of TiO2-tipped Au nanobipyramids (NBPs) to give (Au NBP)/t-TiO2 nanodumbbells. The surfactant cetyltrimethylammonium bromide concentration is the key factor in the construction of this type of unique nanostructure. The photocatalytic aerobic oxidative coupling of amines using the plasmonic photocatalysts with the dumbbell-like and core@shell structures indicates that the TiO2-tipped ends for the photo-reduction and the exposed adjacent Au surface for the photo-oxidation on (Au NBP)/t-TiO2 can significantly improve the photocatalytic activity. The underlying mechanism of the photocatalytic oxidative coupling of benzylamine over (Au NBP)/t-TiO2 has been thoroughly investigated. Both experimental and simulation results for (Au NBP)/t-TiO2 and (Au nanorod)/t-TiO2 confirm the important effect of the plasmonic hotspots on the enhancement of the photocatalytic activity.
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Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 23
·5261-5267
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IF 6.813
Ke Guo,Guang'an Jie,Jiahui Liu,Yanghe Fu,Rui Ma,Xinqing Lu,Fumin Zhang,Weidong Zhu,Maohong Fan
Photocatalytic selective oxidation in organic synthesis has been emerging as an environmentally friendly and energy sustainable approach to produce valuable chemicals, yet it remains a great challenge. In this study, a vanadium(IV) metal–organic framework constructed from triphenyl-based organic linkers, named BIT-66, was first employed as a photocatalyst for the selective oxidation of amines and sulfides in the presence of molecular oxygen or tert-butyl hydroperoxide (TBHP). BIT-66 possesses efficient visible-light absorption and photoinduced charge generation properties, and exhibits an excellent photocatalytic performance for oxidation reactions to produce valuable imines or sulfoxides with a high selectivity under visible light, as well as good reusability. The reactive oxygen species were further investigated via lots of quenching experiments and electron paramagnetic resonance trapping measurements for photocatalytic reactions. It is found that the superoxide radicals, resulting from the photogenerated electron transfer of the excited BIT-66, could be the main active species in the oxidative coupling of amines, while both hydroxyl and peroxyl radicals together play crucial roles in the oxygenation of sulfides using TBHP as the oxidant. This study demonstrates the great potential of photoactive MOFs for organic transformations to produce valuable chemicals.
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ANALYTICA CHIMICA ACTA
·
2022
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IF 6.911
Ruiming Chen,Tingting Hu,Shu Xing,Tao Wei,Jianbin Chen,Tianduo Li,Qingfen Niu,Zhengyang Zhang,Huijun Ren,Xiaoxu Qin
Hydrazine (N 2 H 4 ) and hypochlorite (ClO − ) are extremely harmful to the public health, so it is vitally necessary to detect them in living system. Herein, we developed a new phenthiazine-thiobarbituric acid based dual-analyte responsive fluorescent sensor PT for visually distinguishing and detecting N 2 H 4 and ClO − . PT underwent N 2 H 4 /ClO − -induced C C breakage, achieving olive-drab/brilliant green fluorescence lighting-up response towards N 2 H 4 /ClO − with superb specifity, ultra-sensitivity (detection limit: 15.4 nM for N 2 H 4 , 13.7 nM for ClO − ), and ultra-fast response (N 2 H 4 : <15 s, ClO − : <20 s). The mechanisms for sensing N 2 H 4 and ClO − were investigated with support of spectral measurements and DFT investigation. Sensor based paper-strip/silica-gel device was developed for in-field supervision and on-site monitoring of gaseous and aqueous N 2 H 4 and ClO − solution. In addition, the PT was also applied for quantitatively detecting N 2 H 4 and ClO − in soil, food, plants and bio-fluids. Moreover, PT was utilized to visualize exogenous N 2 H 4 and ClO − in living plants and live-cells, demonstrating this sensor utilized as a powerful tool to detect N 2 H 4 and ClO − in biological fields.
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JOURNAL OF SOLID STATE CHEMISTRY
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2023
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IF 3.3
Shuang Chen,Yin Zhu,Xiaopeng Wei,Guoyuan Zheng,Qiule Zhao,Shuyi Mo,Jilin Wang,Disheng Yao,Nan Tian,Fei Long
A novel bismuth-based zero-dimensional organic-inorganic hybrid material (C 6 H 5 CH 2 NH 3 ) 2 (CH 3 CH 3 NH 2 ) 3 Bi 2 Br 11 was synthesized by a hydrothermal method . The crystal structure, intermolecular interactions , chemical groups, chemical bond characterization, optical and thermal stability of the sample were systematically investigated by single crystal X-ray diffraction, powder X-ray diffraction, Hirshfeld surface analysis, field scanning electron microscopy, Fourier transform infrared spectrometer, Raman spectra , thermogravimetric analysis , and Ultraviolet–visible diffuse reflectance spectra. The results indicated that the (C 6 H 5 CH 2 NH 3 ) 2 (CH 3 CH 3 NH 2 ) 3 Bi 2 Br 11 crystal displayed a triclinic crystal system with a P-1 space group at room temperature with a = 8.5290(4) Å, b = 14.2484(10) Å, c = 18.9386(10) Å, α = 94.418(5) °, β = 102.260(4) °, γ = 106.595(5) °, V = 2131.9(2) Å 3 , Z = 2, R 1 = 0.0936, w R 2 = 0.1536. The compound displayed typical zero-dimensional consisting of two benzylamine organic [C 6 H 5 CH 2 NH 3 ] + cations, three dimethylamine organic [CH 3 CH 3 NH 2 ] + cations and a corner-sharing dimer unit [Bi 2 Br 11 ] 5– . Infrared and Raman vibrational study indicates the presence of [CH 3 CH 3 NH 2 ] + . The 2D fingerprint plot of Hirshfeld surface analysis shows that H⋯Br/Br⋯H (56.8 %) and H⋯H (31.4 %) are major contributions to the intermolecular contact of (C 6 H 5 CH 2 NH 3 ) 2 (CH 3 CH 3 NH 2 ) 3 Bi 2 Br 11 . The sample presented relatively perfect thermal stability up to 240 °C and a wide band gap of about 2.75 eV. It provides some reference value for exploring organic-inorganic hybrid materials with low toxicity and high thermal stability.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Yan Yuandong,Wang Ruyi,Zheng Qian,Zhong Jiaying,Hao Weichang,Yan Shicheng,Zou Zhigang
A thorough comprehension of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, we find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a nonredox process. This nonredox trivalent nickel exhibits exceptional kinetic efficiency in oxidizing organics that possess the highest occupied molecular orbital energy levels ranging from −7.4 to −6 eV (vs. Vacuum level) and the dual local softness values of nucleophilic atoms in nucleophilic functional groups, such as hydroxyls (methanol, ethanol, benzyl alcohol), carbonyls (formamide, urea, formaldehyde, glucose, and N-acetyl glucosamine), and aminos (benzylamine), ranging from −0.65 to −0.15. The rapid electrooxidation kinetics can be attributed to the isoenergetic channels created by the nucleophilic attack and the nonredox electron transfer via the unoccupied e g orbitals of trivalent nickel (t 2g 6 e g 1 ). Our findings are valuable in identifying kinetically fast organic electrooxidation on nonredox catalysts for efficient energy conversions.
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MACROMOLECULES
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2023
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IF 5.5
Hao Liu,Xiangmin Ding,Min Lin,Ronald N. Zuckermann,Jing Sun
Fabrication of functional anisotropic polymeric nanostructures is of great interest and enables a wide range of applications such as protein crystallization. In this sense, we prepared a series of supramolecular nanostructures bearing different surface charges, including star-like superstructures and two-dimensional (2D) nanosheets from diblock copolymers containing crystalline polypeptoids via a hierarchical assembly strategy in a one-pot preparation. We demonstrate that the star-like structures possess a central core with less ordered polypeptoid chains and crystalline emanated branches with oriented molecular packing by grazing incidence wide-angle X-ray scattering (GIWAXS). Further, we developed a new strategy to apply the obtained polypeptoid-based superstructures for the promotion of the nucleation and growth of four types of protein crystals over a wide range of isoelectric points. To the best of our knowledge, this is the first report utilizing protein-mimetic supramolecular structures to efficiently promote the growth of protein crystals. Notably, the protein crystal quantity and quality are greatly improved by the addition of supramolecular nanostructures. In addition, the heterogeneous nucleation has been greatly enhanced, as indicated by the increased heterogeneous nucleation rate (Nhetero). The maximum Nhetero can reach up to 14 with the amine-containing nanostructures, larger than previously reported values. We demonstrate that protein crystal growth is highly dependent on the surface charge of the nanostructures. Such a broadly applicable approach presents great potential in protein crystallization for biotechnological applications.
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Small
·
2023
·
IF 13.3
Zeng-Kui Zhu,Tingting Zhu,Shihai You,Panpan Yu,Jianbo Wu,Ying Zeng,Qianwen Guan,Zhou Li,Chang Qu,Haiqing Zhong,Lina Li,Junhua Luo
Lead halide hybrid perovskites have made great progress in direct X-ray detection and broadband photodetection, but the existence of toxic Pb and the demand for external operating voltage have severely limited their further applications and operational stability improvements. Therefore, exploring “green” lead-free hybrid perovskite that can both achieve X-ray detection and broadband photodetection without external voltage is of great importance, but remains severely challenging. Herein, using centrosymmetric (BZA) 3 BiI 6 ( 1 , BZA = benzylamine) as a template, a pair of chiral-polar lead-free perovskites, (BZA) 2 ( R / S -PPA)BiI 6 ( 2- R / S , R / S -PPA = ( R / S )-1-Phenylpropylamine) are successfully obtained by introducing chiral aryl cations of ( R / S )-1-Phenylpropylamine. Compared to 1 , chiral-polar 2- R presents a significant irradiation-responsive bulk photovoltaic effect (BPVE) with an open circuit photovoltage of 0.4 V, which enables it with self-powered X-ray, UV–vis-NIR broadband photodetection. Specifically, 2- R device exhibits an ultralow detection limit of 18.5 nGy s −1 and excellent operational stability. Furthermore, 2- R as the first lead-free perovskite achieves significant broad-spectrum (377–940 nm) photodetection via light-induced pyroelectric effect. This work sheds light on the rational crystal reconstruction engineering and design of “green” hybrid perovskite toward high-demanded self-powered radiation detection and broadband photodetection.
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Polymers
·
2023
·Vol. 15
·期 20
·4145
·
IF 5
Guichuan Xu,Zhuhan Wang,Yefeng Chen,Li Qin,Limei Zhou
Porous carbon nitride/bismuth oxychloride (PCN/BiOCl-x) polymer-based heterojunction photocatalysts were successfully synthesized via a simple in situ hydrothermal method. A PCN/BiOCl heterojunction with rich chlorine defects is prepared by adjusting the chlorine content of the BiOCl unit in the heterojunction by changing the solvent. The as-prepared catalysts were characterized via BET, SEM, TEM, XRD, XPS and optical testing, and they were used for a photocatalytic amine oxidation reaction. The results indicated that the catalytic performance of the PCN/BiOCl heterojunction was significantly enhanced due to the rich chlorine vacancies in the samples. The enhanced catalytic activity may be attributed to the Z-scheme heterojunction, abundant chlorine defects and large specific surface area. At the same time, the catalyst circulation experiment shows that the PCN/BiOCl heterojunction has good circulation performance.Keywords:chlorine vacancy;Z-scheme heterojunction;amine oxidation;polymer-based;photocatalysis
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CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 35
·7955-7960
·
IF 4.857
Bingquan Jia,Du Sun,Wei Zhao,Fangfang Xu,Fuqiang Huang
Graphical Ball control : A new synthetic method based on CdNCN nanoparticle anion exchange reactions was developed to access solid or hollow CdSe nanocrystals with tunable size, which exhibit narrow width of photoluminescence features. The obtained CdNCN@CdS heterostructures with modulated shell/core thickness show a remarkable improvement in photocatalysis compared to CdS or CdNCN NPs of similar size. Semiconductor nanocrystals of tunable shell/core configurations have great potential in photo-driven applications such as photoluminescence and photocatalysis, but few strategies realize a controllable synthesis with respect to both the size of the core and the shell with high crystallinity. Here, a new synthetic method based on cadmium cyanamide (CdNCN) nanoparticle anion exchange reactions was developed to access solid or hollow CdSe nanocrystals with tunable size and CdNCN@CdS heterostructures with modulated shell/core thickness. The gradual shift and narrow width of photoluminescence features demonstrate the high crystallinity and monodispersity of the resulting CdSe nanocrystals. In the CdNCN@CdS heterostructures, synergistic effects of the photocarrier separation is observed between the CdS shell and CdNCN core, which leads to great improvement in photocatalysis with optimized shell/core ratio.
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Small
·
2023
·Vol. 19
·期 50
·2304674
·
IF 13.3
Kailai Zhang,Xiaodong Sun,Haijun Hu,Ge Yan,Anqi Qin,Yali Ma,Hongwei Huang,Tianyi Ma
Mechanical energy driven piezocatalytic hydrogen (H 2 ) production is a promising way to solve the energy crisis . But limited by the slow separation and transfer efficiency of piezoelectric charges generated on the surface of piezocatalysts , the piezocatalytic performance is still not satisfactory. Here, defect engineering is first used to optimize the piezocatalytic performance of microcrystalline cellulose (MCC). The piezocatalytic H 2 production rate of MCC with the optimal defect concentration can reach up to 84.47 µmol g −1 h −1 under ultrasonic vibration without any co-catalyst, which is ≈3.74 times higher than that of the pure MCC (22.65 µmol g −1 h −1 ). The enhanced H 2 production rate by piezoelectric catalysis is mainly due to the introduction of defect engineering on MCC, which disorders the symmetry of MCC crystal structure, improves the electrical conductivity of the material, and accelerates the separation and transfer efficiency of piezoelectric charges. Moreover, the piezocatalytic H 2 production rate of MCC with the optimal defect concentration can still reach up to 93.61 µmol g −1 h −1 in natural seawater, showingits commendable practicability. This study presents a novel view for designing marvelous-performance biomass piezocatalysts through defect engineering, which can efficiently convert mechanical energy into chemical energy .
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Cong Geng,Yanxing Feng,Quanlin Chen,Yuanzhi Jiang,Saif M. H. Qaid,Mingjian Yuan
Organic–inorganic halide perovskite single crystals with exceptional optoelectronic properties have become some of the most promising candidates for ionizing radiation detection. However, the existence of ion migration could cause collapse of the crystal interior and still hinder the realization of stable detection devices. As the most economical and convenient way to obtain large single crystals, the traditional inverse temperature crystallization (ITC) method with an accelerating growth pathway could induce the generation of more defects and aggravate the ion migration. In this study, we formulated a strategy to mitigate the growth acceleration phenomenon by incorporating an intermediate state within the ITC system through the introduction of benzylammonium iodide (BAI). BAI is capable of coordinating with the perovskite crystal's surface, thereby retarding the pace of growth. The grown single crystal of MA0.9GA0.1PbI3 (MA = methylammonium, GA = guanidinium) shows optimized defect density with the ion migration suppressed successfully. The fabricated X-ray detection device demonstrates an outstanding sensitivity of 9.19 × 105 μC Gyair–1 cm–2 and exceptional stability. It exhibits a remarkably low dark current drift of 4.50 × 10–7 nA cm–1 V–1 s–1 under a high bias of 330 V/cm during continuous operation over 30,000 s. This reduction is nearly 1 order of magnitude compared to other methods. Moreover, the device achieves a 3-fold enhancement in X-ray dose tolerance while maintaining 80% of its original sensitivity.
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