CARBON
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2022
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IF 11.307
Xiang Yu,Yue Zhan,Tingting Fan,Yuqi Zhang,Shunqin Liang,Limin Sun,Xiaoli Hu,Weiping Fang,Zhou Chen,Xiaodong Yi
The stabilization and transport of the reactants, intermediates and products are significant to rational design of an industrial catalyst. In this work, we encapsulated the surface of Pd/g-C 3 N 4 catalyst with acrylic acid (AA) using a photo-induced grafting method to mimic the 3-dimensional nature of enzymes. A combined characterization and ab initio calculation revealed that AA ligands on the surface controlled the adsorption and diffusion behaviors of the reactants, rather than alter the electronic or geometric properties of Pd active centers. The optimized catalyst (Pd/CNA-4) significantly enhances isoprene partial hydrogenation activity without a decline in semi-hydrogenation selectivity. This approach can be further optimized by changing the types of the encapsulating ligands and can meet other specific catalytic reactions to regulate their conversion and selectivity and is therefore expected to extend to other areas of heterogeneous catalysis .
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BIOELECTROCHEMISTRY
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2022
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IF 5.76
Xianhua Shi,Yixuan Xie,Linxi Chen,Jing Lu,Luyong Zhang,Duanping Sun
Zeolitic imidazolate frameworks (ZIFs), a famous subfamily of metal-organic frameworks (MOFs), are considered promising electrocatalysts. Herein, ZIF-67 was selected as an electrocatalyst for designing electrochemical sensors due to having the best electrocatalytic activity in ZIFs. To overcome the insufficient electrocatalytic activity of ZIFs, ZIF-67 derivatives (QZIF-67-X, where X represents calcination time) were obtained by calcining at 250 °C for a certain time. The porous structure of the precursor in QZIF-67-X is maintained, exposing more active centers. QZIF-67-X could accelerate electron transfer and lead to improve the electrocatalytic performance. Moreover, QZIF-67-2 was chosen as an Au nanoparticle-supported nanocarrier to further bind G-quadruplex/hemin DNAzymes with strong catalytic activity due to the best supporting activity of QZIF-67-2 among QZIF-67-X. The synergistic catalysis of QZIF-67-2 and G-quadruplex/hemin DNAzymes effectively amplified the reduction current signal of H 2 O 2 . The linear range of the prepared electrochemical sensor was 2 μM-65 mM, and the detection limit was 1.2 μM. Moreover, the real-time detection of H 2 O 2 from HepG2 cells was achieved by the sensor, providing a novel technique for efficient anticancer drug evaluation. These results suggested that QZIF-67 can be utilized as an efficient electrocatalyst for improving the sensitivity of sensors.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yan Wang,Guangshe Li,Chang Liu,Xinbo Li,Liping Li
Metal geometrical structure engineering of composite catalysts is powerful to boost their photocatalytic performance of hydrogen evolution . Herein, by rationally designing, transition metal phosphides (TMPs) have been loaded onto the P doped g-C 3 N 4 (PCN) to construct catalysts TMPs/PCN. For the first time, the effect of geometrical structure of TMPs on the photocatalytic activity is optimized and a geometrical-site-dependent photocatalytic hydrogen evolution is experimentally determined. Tri-metallic FeCoNiP/PCN, having 59.6% occupancy of tetrahedral cobalt sites, gives hydrogen production rate of 205 μmol/g/h, better than that of mono-metallic (FeP, CoP , NiP), bi-metallic (FeCoP, CoNiP, FeNiP) TMPs/PCN, and even much superior to that of Pt/b-g-C 3 N 4 and Pt/PCN. Trimetallic TMPs/PCN catalysts also show excellent OER performance. In addition to the efficient electron transfer between FeCoNiP and PCN, which can effectively improve the separation of photogenerated carriers, the high occupancy of tetrahedral cobalt sites of FeCoNiP as a co-catalyst promotes the formation of active intermediates, being the key to significantly improve the catalytic performance of ternary FeCoNiP/PCN. The findings in this work, especially about a link of the photocatalytic performance of TMPs/PCN composites and occupancy of tetrahedral cobalt site in co-catalysts TMPs, can open new occasion for creating novel composite catalysts and extending to other applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jiangfu Zheng,Changzheng Fan,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Shuaijun Pan,Baowei Zhang,Jinglin Ding,Shengxiang Rong,Haoyu Yin
Development of efficient nanomaterials for photocatalytic degradation is very important in the removal of organic pollutants from water. The oxygen vacancy-rich g-C 3 N 4 / LDH composites (g-C 3 N 4 /LDH-OVs) with a layered structure was prepared for the efficient photocatalysis degradation and mineralization of tetracycline hydrochloride (TC) under visible light irradiation. Oxygen vacancies in the composites achieved through structural induction strategy not only provide abundant active sites but also improve the separation efficiency of the photo-generated carriers, thereby enhancing the degradation and mineralization of TC, as revealed both by theories and experiments. The optimized g-C 3 N 4 /LDH-OVs have achieved excellent photocatalytic activity (i.e., 95 % degradation and 28 % mineralization of TC after 60 min of visible light irradiation), which was 2.3 and 3.5 times higher than that of the pristine g-C 3 N 4 and LDH-OVs, respectively. Furthermore, experimental results based on bio-acute toxicity show that the g-C 3 N 4 /LDH-OVs/Vis system can effectively detoxify the transformation products. This study provides an insight into the development of LDH-based photocatalysts, so as to realize photocatalytic mineralization and simultaneous detoxification through the new strategy of oxygen vacancy defect engineering.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Shangyuan Ni,Zhengrong Fu,Lin Li,Manying Ma,Yuelin Liu
Construction of heterojunction between semiconductors is considered an effective strategy for enhancing photocatalytic capability. Herein, this work prepared an abundant porous g-C 3 N 4 /TiO 2 photocatalyst , with the two-dimensional (2D) nanosheet g-C 3 N 4 and nanoparticle TiO 2 . The heterojunction both enhanced the ultraviolet (UV) light absorption ability, and inhibited the recombination of photogenerated electron-hole (h + ) pairs. As expected, the optimal 4 % g-C 3 N 4 /TiO 2 (g-C 3 N 4 :TiO 2 = 1:25) exhibited a prominent degradation efficiency of 96.53 % in the photocatalytic performance of tetracycline hydrochloride (TCH) under UV irradiation . The recycling of the heterojunction photocatalyst g-C 3 N 4 /TiO 2 remained stability and reusability. The main active species were·O 2- , h + and·OH, and the formation of internal electric field on the step-scheme (S-scheme) heterojunction interface accelerated the migration of photogenerated carriers. Moreover, several environmental factors on degradation such as dose, pH, and the initial concentration of TCH were investigated. This work could be spread to the conceive of other S-scheme heterojunction photocatalysts in application to different environmental demands.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jinxing Hou,Guodong Dai,Jiuwu Wang,Xian Sun,Yue Situ,Hong Huang
A novel ternary polythiophene/Ag/protonated g-C 3 N 4 nanosheets (PTh/Ag/pCN) nanocomposite was constructed by electrostatic self-assembly strategy. The as-prepared 5% PTh/Ag/pCN exhibits excellent visible light photocatalytic performance toward methylene orange (MO), which is 6 and 3.7 times higher than pCN and PTh, respectively. The result was dominantly ascribed to the forming of Z-scheme heterojunction due to the synergetic effects of pCN, Ag and PTh, which is conductive to the separation of photogenerated charges. Meanwhile, the radical trapping experiments and ESR techniques proved that the photogenerated holes and superoxide radicals are vital reactive substances. This study provides a powerful approach to enhance catalytic activity of conjugated polymer photocatalyst .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 50
·76404-76416
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IF 5.19
Hu Jie,Lu Songhua,Ma Jianfeng,Zhu Fang,Komarneni Sridhar
In this paper, the g-C 3 N 4 /ZnIn 2 S 4 composite was synthesized by a two-stage hydrothermal method. The microstructure, surface, and optical properties of the composite were thoroughly characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET) surface area analysis, and UV-Vis absorption spectroscopic analysis. The removal capacity of Cr(VI) was optimized by using ZnIn 2 S 4 loaded in the composite. Meanwhile, the optimal pH environment for the reduction of Cr(VI) was determined to be about pH 3, and the reduction efficiency could reach more than 99% within 60 min. Further, the results of UV-Vis absorption analysis indicated the high and wide range of light absorption by composite compared with pure g-C 3 N 4 . Therefore, the enhanced photocatalytic performance of the composite could be attributed to the well-matched energy band structure between g-C 3 N 4 and ZnIn 2 S 4 , which apparently promoted the effective separation and transfer of photogenerated carriers. In addition, the composite showed good stability in the visible light catalytic reaction, and the possible mechanism of the photocatalytic activity of Cr(VI) reduction by the composite was proposed.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
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IF 5.141
Qiusha Li,Shuzhen Peng,Yun Chang,Mujing Yang,Dandan Wang,Xiaoshun Zhou,Yong Shao
G-triplex (G3), as an intermediate of G-quardruplex (G4), is a typical non-classical DNA topology with three G-tracts, formed by folding guanine-riched DNA sequences. The flexibility and tunability of G3-folding structures can provide a versatile platform for analytes sensing. However, current researches about G3s on sensing applications, especially on metal ion sensing, are relatively rare. Herein, we first develop a label-free fluorescence switch-on sensing platform based on the G-triplex topology (HtG3) for the specific qualitative identification of chromium species. Coralyne (COR), a molecule probe whose fluorescence can be inhibited by HtG3, is employed to monitor the Cr 3+ binding events with the principle that Cr 3+ could break the parallel HtG3-folding structure to result in COR releasing from HtG3 and its fluorescence recovery. Furthermore, this HtG3 sensing platform we constructed also can be used to indirectly identify CrO 4 2- through reducing it to Cr 3+ with ascorbic acid (AA). Our work will extend the practical application of G3 as a biosensor and inspire wide interests in exploring more non-classical DNA structures.
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JOURNAL OF ELECTRONIC MATERIALS
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2022
·Vol. 51
·期 10
·5508-5520
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IF 2.047
Wang Yan,Zheng Zhanshen,Li Yuanliang,Jia Pengwei,Liu Tong
Degradation of harmful pollutants is the key to water pollution control. Herein, a series of BiOI/g-C 3 N 4 -Ag 2 O (BCNA) heterojunction photocatalysts were prepared by a simple liquid-phase synthesis method for photocatalytic degradation of organic pollutants under visible light. The crystal structure, morphology, and elemental composition of the synthesized photocatalysts were characterized by x-ray diffractometer (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), and x-ray photoelectron spectroscopy (XPS). The experimental results showed that compared with g-C 3 N 4 and BiOI, BiOI/g-C 3 N 4 -Ag 2 O composite showed the best photocatalytic activity when the Ag 2 O loading was 14.68 wt.%, and the removal rate of rhodamine B (RhB) could reach 98% after 30 min, and the photodegradation showed good stability through the cycle tests. In addition, UV–Vis diffuse reflectance spectroscopy (UV–Vis DRS), photoluminescence excitation spectrum (PL), and photoelectrochemical measurements confirmed that the enhanced photoactivity of BiOI/ g-C 3 N 4 -Ag 2 O is due to the formation of ternary heterojunction, which not only amplifies the visible light response of g-C 3 N 4 but also improves the separation and migration rate of photoinduced carriers. Finally, a possible mechanism of charge separation and transfer for ternary heterojunction photocatalysts was proposed. This study extends the application range of g-C 3 N 4 for RhB degradation and provided a new opportunity for environmental remediation.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 20
·6149-6156
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IF 4.478
Qin Shanshan,Chen Xuliang,Xu Zhichen,Li Tao,Zhao Shuhong,Hu Rui,Zhu Jiang,Li Ying,Yang Yunhuang,Liu Maili
Few reports are found working on the features and functions of the human telomere G-triplex (ht-G3) though the telomere G-quadruplex has been intensely studied and widely implemented to develop various biosensors. We herein report that ht-G3 lights up Thioflavin T (ThT) and establish a sensitive biosensing platform for RNA detection by introducing a target recycling strategy. An optimal condition was selected out for ht-G3 to promote ThT to generate a strong fluorescence. Accordingly, an ht-G3-based molecular beacon was successfully designed against the corresponding RNA sequence of the SARS-CoV-2 N-gene. The sensitivity for the non-amplified RNA target achieves 0.01 nM, improved 100 times over the conventional ThT–based method. We believe this ht-G3/ThT–based label-free strategy could be widely applied for RNA detection.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
P. Velusamy,Shanhu Liu,Ruimin Xing,M. Sathiya,Awais Ahmad,Munirah D. Albaqami,Reham Ghazi Alotabi,Elangovan Elamurugu,M. Senthil Pandian,P. Ramasamy
Due to their superior optoelectronic characteristics and affordable cost, doped few-layered g-C 3 N 4 (FCN) semiconductor nanostructures are attractive for photocatalytic and photoelectrochemical (PEC) water splitting applications. Nano heterostructures composed of Praseodymium (Pr)-doped few-layered graphitic carbon nitrides (FCN) and bismuth oxy iodide (BiOI) are manufactured using thermal condensation and hydrothermal technique in two steps. The inclusion of Pr dopant not only modifies the FCN by increasing its porosity and specific surface area, but also improves electron-hole separation and charge transfer. The metal-free nano heterostructure (Pr: FCN/BiOI) that was created exhibits a strong electron-hole separation. The observed rapid charge transit in a heterojunction results in a low rate of charge recombination. Thus, the produced metal-free nano heterostructure overcomes the barrier of FCN's high photo-charge carrier recombination rate. This study investigates the influence of Pr-doping on the structural, optical, electrical conductivity , and PEC characteristics of produced heterostructures. The addition of Pr dopant to FCN increases its ability to absorb solar light. The photocurrent density of the 1.5 wt percent Pr: FCN/BiOI nano heterostructure is 16.8 times greater than that of the 1.5 wt percent Pr: FCN nanostructure. In comparison to the other Pr-doping doses, it exhibits a high hydrogen evolution reaction (HER) photocurrent density (18.21 mA/cm 2 ) and hydrogen evolution rate (3400 mol h −1 cm −2 ) under solar light irradiation (420 nm). The current work gives significant insight into the optimization of composition and structural features for FCN photoelectrocatalysis with excellent performance.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Kailin Wang,Songyu Yang,Yan Wu
Dual cocatalysts play an important role in photocatalytic water splitting to hydrogen production . In this paper, Fe-doped Co 3 O 4 (Fe-Co 3 O 4 ) and Pt were loaded on the surface of g -C 3 N 4 to enhance the water photocatalytic splitting, in which Fe-Co 3 O 4 was used as an oxidation cocatalyst to capture the photo-generated holes of g -C 3 N 4 , and Pt was used as a reduction cocatalyst to transfer photo-generated electrons. Under the irradiation of visible light, its hydrogen production rate reaches up to 3.015 mmol g −1 h −1 , which is 3.01 times higher than that of g -C 3 N 4 loaded with Pt. Pt and Fe-Co 3 O 4 dual cocatalysts not only promote the migration rate of photo-generated electrons and holes on the surface of g -C 3 N 4 , but also improve the light absorption capacity of visible light. The interfacial electric field built from the p-n heterojunction of Fe-Co 3 O 4 / g -C 3 N 4 drives photo-generated electrons in Fe-Co 3 O 4 flowing to the holes of g -C 3 N 4 , which further inhibiting the recombination of g -C 3 N 4 photo-generated carriers. This work provides a reference for the development of high-efficiency photocatalyst and an effective support for the development of semiconductor cocatalyst.
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