APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Lei Chen,Yiming Xu,Zhi Yang,Kun Zhang,Baoliang Chen
Developing a low-cost co-catalyst for hydrogen evolution reaction (HER) on a photocatalyst is a great challenge. An open-framework material, cobalt ethylenediammonium bis(sulfate) tetrahydrate, was initially used as an efficient co-catalyst to improve photocatalytic HER of g-C 3 N 4 . The unique open‐framework cobalt(II) sulfate (Co-S) lead to twice higher H 2 evolution performance (10328.9 μmol g −1 h -1 ) compared to noble metal (Pt)-decorated g-C 3 N 4 photocatalyst under simulated sunlight. The open network structure provides abundant active sites and excellent electron transport properties, properties and then promotes electron-hole separation, which play a synergistic role with g-C 3 N 4 in the photocatalytic process. The loading of Co-S significantly changes the microenvironment of the catalyst surface of g-C 3 N 4 and enhances its hydrophilicity, which benefits the release of the produced gas on the catalyst surface. The formation of the Co(Ⅰ) species in the open-framework material by the electron reduction of Co(Ⅱ) is proposed as a vital role in the extraordinary HER process.
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FUEL
·
2020
·
IF 5.578
Yong-Ting Li,Xiao-Li Zhang,Zhi-Kun Peng,Pu Liu,Xiu-Cheng Zheng
The hydrolysis of solid storage compounds including ammonia borane (NH 3 BH 3 ) is promising for the upcoming hydrogen economy. So, developing highly efficient heterogeneous catalysts for the hydrolysis of ammonia borane is one of the key issues since this reaction is not kinetically feasible at room temperature. In this work, a facile adsorption- in situ reduction method is adopted to stabilize the ultrafine bimetallic RuPd nanoparticles on an ultrathin porous graphite carbon nitride. Due to the synergistic alloying effect, most of the resultant bimetallic Ru 1- x Pd x /g-C 3 N 4 catalysts possess much higher catalytic activity than the monometallic Ru/g-C 3 N 4 and Pd/g-C 3 N 4 in the hydrolytic dehydrogenation of ammonia borane. Catalyzed by the optimal Ru 0.85 Pd 0.15 /g-C 3 N 4 , the turnover frequency and the apparent activation energy are 948.2 mol H 2 ·mol Cat -1 ·min - 1 and 24.2 kJ mol −1 , respectively, which are much superior to many catalysts previously reported. The high catalytic activity and satisfactory durability endow Ru 0.85 Pd 0.15 /g-C 3 N 4 desirable potential in the hydrogen generation from the hydrolysis of chemical storage materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Zhiyuan Zhou,Dong Yang,Wenjing Wang,Yao Chen,Zhanfeng Zhao,Ke An,Hanjie Ren,Zhongyi Jiang
Graphite-like carbon nitride (CN) has attracted much attention because of its distinct optical and photoelectrical properties, strong stability, and wide applications for environmental restoration and renewable energy. Herein, the CN nanolayer about 7.5–17.5 nm in thickness was in situ built uniformly on the external of carbonized PDA (cPDA) spheres to form the cPDA@CN core/shell nanomaterials on account of the bioinspired adhesion. They possess the mesopore about 4.8 nm in diameter and a high specific surface area (66.6 m2 g–1). The optimal cPDA@CN sample exhibits efficient catalytic activities for the rhodamine B degradation (2.19 h–1) and H2 release rate (630 μmol g–1 h–1), which are ∼15.4 and ∼10 times of pristine CN, respectively. This research affords a dextrous and scalable way to fabricate the nanostructured photocatalyst with superior performance, which may hold great promise in practical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Lu Zhang,Meng Zhang,Xiaozhe Song,Hui Wang,Zhaoyong Bian
Here, we report enhancement of the photoelectrochemical (PEC) performance of MnO x /graphite-like carbon nitride (g-C 3 N 4 ) nanocomposites synthesized by one-step thermal decomposition for degradation of clofibric acid (CA). MnO x showed enhanced broadband ultraviolet–visible light regions, efficient charge generation–separation, and enhanced PEC performance when combined with g-C 3 N 4 . Photogenerated holes can be efficiently captured by introducing Mn 2+ /Mn 3+ /Mn 4+ valence band transitions. In addition to a good visible-light response, the MnO x /g-C 3 N 4 -10 (g-C 3 N 4 with 10% Mn(NO 3 ) 2 ·6H 2 O) photoanode showed enhanced photocurrent density of 0.03 × 10 −3 A cm −2 at 0.63 V vs. Ag/AgCl, which was approximately 100 times that of pristine g-C 3 N 4 . The superoxide radical and positive holes played dominant roles in PEC degradation of CA. The MnO x /g-C 3 N 4 -10 photoanode showed the highest photoelectrocatalytic performance under acidic conditions because of electrostatic attraction between the electrode and CA. The CA degradation ratio using the MnO x /g-C 3 N 4 -10 photoanode was 100% under visible light in 6 h at pH = 3. This work provides a simple and sustainable strategy to modify g-C 3 N 4 for captured holes to improve PEC degradation of CA, and it is promising for application to different materials in a variety of fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
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IF 5.774
Bin Zhang,Xu He,Xiaohan Ma,Qinghua Chen,Guocheng Liu,Yuanming Zhou,Dong Ma,Chunyue Cui,Jun Ma,Yanjun Xin
To improve the redox performance and light absorption property, the 2D/0D g-C 3 N 4 /TiO 2 heterojunction photocatalyst were successfully fabricated by co-annealing process based on melamine powder and ultrafine TiO 2 nanoparticles (about 9.87 nm) obtained from electrochemical etching technology. The surface micromorphology, crystal structure, basic element composition, chemical structure, specific surface and optical performance were analyzed by SEM-EDS, TEM, HR-TEM, XRD, XPS, FTIR and Ultraviolet–visible diffuse reflection spectra (UV–vis DRS). The photocatalytic performance of g-C 3 N 4 /TiO 2 photocatalyst was assessed by the degradation of tetracycline hydrochloride (TC) under simulated sunlight irradiation. The results showed that the obtained TiO 2 powder had extremely smaller particle size and higher photocatalytic activity than commercial P25. The coupling of 0D TiO 2 nanoparticles and 2D g-C 3 N 4 nanosheet further promoted the visible light absorption performance of TiO 2 . The unique g-C 3 N 4 /TiO 2 heterojunction photocatalyst exhibited remarkable photocatalytic performance for the degradation of TC, whose degradation rate could reach to 99.40% under 120 min irradiation. The kinetic constant of the g-C 3 N 4 /TiO 2 photocatalyst was 1.48 times of that of TiO 2 . The ESR results confirmed ·OH and ·O 2 – radicals produced in the photocatalytic process. This work could provide an effective reference for the fabrication of ultrafine TiO 2 powder and binary heterojunction photocatalyst with excellent photocatalytic activity for organic pollutants degradation in water purification.
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RSC Advances
·
2020
·Vol. 10
·期 28
·16515-16525
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IF 3.119
Junya Cao,Fenggang Han,Liguo Wang,Xiaoyu Huang,Yan Cao,Peng He,Huanhuan Yang,Jiaqiang Chen,Huiquan Li
A series of Ru/g-C3N4 materials with highly dispersed Ru were firstly prepared by an ultrasonic impregnation method using carbon nitride as a support. The catalysts were characterized by various techniques including BET and elemental analysis, ICP-AES, XPS, XRD, CO2-TPD and TEM. The results demonstrated that Ru/g-C3N4 materials with a mesoporous structure and highly dispersed Ru were successfully prepared. The chemo-selective hydrogenation of p-phenylenediamine (PPDA) to 1,4-cyclohexanediamine (CHDA) over Ru/g-C3N4 as a model reaction was investigated in detail. PPDA conversion of 100% with a CHDA selectivity of more than 86% could be achieved under mild conditions. It can be inferred that the carbon nitride support possessed abundant basic sites and the Ru/g-C3N4-T catalysts provided suitable basicity for the aromatic ring hydrogenation. Compared to the N-free Ru/C catalyst, the involvement of nitrogen species in Ru/g-C3N4 remarkably improved the catalytic performance. In addition, the recyclability of the catalyst demonstrated that the aggregation of Ru nanoparticles was responsible for the decrease of the catalytic activity. Furthermore, this strategy also could be expanded to the selective hydrogenation of other aromatic diamines to alicyclic diamines.
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高影响因子
CARBON
·
2019
·
IF 7.466
Wei Miao,Ying Liu,Xiaoyan Chen,Yixin Zhao,Shun Mao
In recent years, design high catalytic graphitic carbon nitride (g–C 3 N 4 )–based catalysts has drawn broad attention in environmental remediation. In this work, a series of iron-doped g-C 3 N 4 compounds were synthesized through a simple bottom-up strategy. By controlled pyrolysis , iron-doped g-C 3 N 4 materials split from bulk structure into multi-layer structure with uniformly dispersed mesopores. The catalytic activities of layered iron-doped g-C 3 N 4 in Fenton-like and photo-Fenton-like processes were investigated. Due to the doped iron, unique layered structure, and mesopore feature, the catalysts present greatly enhanced performance in heterogeneous Fenton-like reactions. Moreover, the degradation parameters calculated by the pseudo-first-order kinetic model fitted well with the specific surface area of the catalyst, indicating that the catalytic activities rely heavily on the specific surface area of layered and porous g-C 3 N 4 . This study presents a facile and generic method to regulate C 3 N 4 morphology and structure for enhanced catalytic activity in Fenton-like reactions.
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Rui Liu,Bin Kong,Yun Chen,Xueping Liu,Shengli Mi
The helical structure is one of the most intriguing structures in nature; such an ingenious structure can be found from macromolecules to macroscopic areas, and the fabrication of helical structures has attracted research interest from mechanisms to applications. However, the fabrication of helical microfiber still remains a big challenge. In this study, a coaxial microfluidic device was made to continuously and controllably fabricate helical hydrogel microfibers with flexible shape by simply adjusting the flowrates. Various experimental conditions that can influence the diameter (d), pitch (p) and amplitude (A) of these formed coiled fibers were discussed. For the first time, the effects of G/M ratio of the alginates on the microfiber coiling phenomenon were examined. Additionally, magnetically responsive helical fibers were synthesized, and it is envisioned that hydrogel helical structure microfibers are highly versatile in different area, such as micro sensors, soft actuators and medical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Ming Lei,Zhiying Wang,Lihua Zhu,Wenshan Nie,Heqing Tang
Deep debromination of polybrominated diphenyl ethers (PBDEs) by visible light photocatalysis is still a challenge in the field of halogenated pollutants control. Here, an efficient photocatalyst (Pd/g-C 3 N 4 ) was prepared by a simple impregnation-chemical reduction method with bulk g-C 3 N 4 and PdCl 2 as precursors. Under preferred reaction conditions (visible light irradiation for 120 min), the use of the 0.5% Pd/g-C 3 N 4 composites (0.4 g L −1 ) yielded an almost complete debromination of BDE47 (10 μmol L −1 ) in methanol-water mixture, while the debromination of BDE47 did not occur on pure g-C 3 N 4 . A “Pd-promoted active H atom species attack and C-Br bond cleavage” route was proposed according to the identified degradation intermediates. A catalytic mechanism was further clarified: Pd nanoparticles exerted affinity interaction with bromine atoms, and the storing of electrons on Pd would increase the binding interaction. In the debromination process, methanol acts as both a hole scavenger and a hydrogen donor to provide active H atom species through the reaction of H + and photogenerated electrons on Pd nanoparticles. The initiation of BDE47 debromination on Pd nanoparticles required an induction period to enrich a critical amount of electrons for stretching the C-Br bond and its subsequent being attacked by active H atoms. The generated 2,2′-dibromodiphenyl ether (BDE4) would be further reduced to bromine-free products by hydro-debromination process or coupling reaction.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Wei Wang,Jiaojiao Fang
Semiconductor-based heteronanostructures with wide light absorption and efficient electron-hole separation properties exhibit great potential for photocatalytic applications. Here we employ the mesoporous SiO 2 nanoparticles as the template to simultaneously exfoliate the nano-confined g-C 3 N 4 and deposit the CdS nanoparticles to form a series of core-shell SiCN@CdS heteronanostructures for photocatalytic H 2 production under the visible light irradiation. Based on the physicochemical characterizations, we have been able to discuss the compositions, structures, and properties of the core-shell photocatalysts . Benefiting from the optimized equilibrium state of a relative high specific surface area, light absorption, crystalline degree, and a homogeneous dispersion of the outer CdS nanoparticles, the SiCN@2CdS exhibits the highest photocatalytic activity and stability for H 2 production under the visible light irradiation. Results also suggest that the existence of the SiO 2 template is benefit to suppress the aggregation and improve the recyclability of the core-shell photocatalysts when they are applied in the aqueous phase. The present study suggests a new sight on the template-assisted designing and synthesizing high-reactive, low-cost, environmental-stable, and easy-recyclable photocatalysts by precisely controlling the microstructures.
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SENSORS
·
2022
·Vol. 23
·期 1
·148
·
IF 3.847
Ji Zhang,Xu Li,Qinhe Pan,Tong Liu,Qingji Wang
Hydrogen (H2) has gradually become a substitute for traditional energy, but its potential danger cannot be ignored. In this study, litchi-like g-C3N4/In2O3composites were synthesized by a hydrothermal method and used to develop H2sensors. The morphology characteristics and chemical composition of the samples were characterized to analyze the gas-sensing properties. Meanwhile, a series of sensors were tested to evaluate the gas-sensing performance. Among these sensors, the sensor based on the 3 wt% g-C3N4/In2O3(the mass ratio of g-C3N4to In2O3is 3:100) showeds good response properties to H2, exhibiting fast response/recovery time and excellent selectivity to H2. The improvement in the gas-sensing performance may be related to the special morphology, the oxygen state and the g-C3N4/In2O3heterojunction. To sum up, a sensor based on 3 wt% g-C3N4/In2O3exhibits preeminent performance for H2with high sensitivity, fast response, and excellent selectivity.Keywords:g-C3N4/In2O3;litchi-like;H2sensor;fast response;high selectivity
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高影响因子
Science China-Materials
·
2022
·Vol. 66
·期 3
·1053-1061
·
IF 8.64
Wang Junxia,Guo Changliang,Jiang Yong,Wan Jiafeng,Zheng Bing,Li Yuxin,Jiang Baojiang
Hydrogen peroxide is an environment-friendly reactive oxygen species and a significant green oxidant. However, the highly efficient and sustainable production of H 2 O 2 remains a challenge. Herein, we demonstrated a state-of-the-art photocatalytic method for H 2 O 2 production using an optimal tubular graphic carbon nitride (TCN)/ZnIn 2 S 4 (ZIS) heterojunction. Within 3 h, a H 2 O 2 production rate of 2.77 mmol g −1 h −1 was achieved by the TCN/ZIS heterojunction, which is 3.4- and 23.1-fold higher than that obtained by its individual TCN and ZIS components, respectively. Experimental results showed that the excellent photoactivity of TCN/ZIS is mainly due to the formation of heterojunction, which improves the charge separation ability and thereby promotes the proton-coupled electron transfer by initially reducing O 2 to ·O 2 − and subsequently generating H 2 O 2 . This work has developed an efficient and green strategy for H 2 O 2 production with scientific and practical value for environmental remediation.
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