DALTON TRANSACTIONS
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2024
·
IF 3.5
Cengceng Du,Zhenyu Wang,Yiming Wang,Wenjuan Xu,Yuqiu Huo,Hongbin Sun,Guangwen Xu
Constructing an environmentally friendly and efficient electrocatalyst holds important and profound significance for energy-efficient hydrogen production. Replacing the oxygen evolution reaction with a lower potential urea oxidation reaction (UOR) may save energy in water electrolysis to produce hydrogen. The UOR is characterized by its high energy barrier, which results in slow reaction kinetics. In this study, we introduced Ba(OH)2 into Ni(OH)2 to form uniform nanosheets. Due to the introduction of Ba2+, the lattice expansion of Ni(OH)2 was triggered, leading to significant improvement in UOR activity. The catalyst achieved a current density of 100 mA cm−2 at only 1.316 V and exhibited remarkable stability over time. Density functional theory (DFT) calculations demonstrate that the Ba–Ni(OH)2 site significantly reduces the energy barrier for urea adsorption, intermediate steps, and desorption. This work provides a novel and environmentally friendly strategy for constructing energy-efficient and highly efficient catalysts through the doping of alkaline earth metals.
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高影响因子
RSC Advances
·
2016
·Vol. 6
·期 55
·50138-50143
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IF 3.289
D. Li,W. B. Li,J. S. Shi,F. W. Xin
Hexagonally packed mesoporous silica (HMS) was used as a kind of template-like material to prepare heteroatom doped porous carbons from the polymerization reactions of resorcinol and formaldehyde in the HMS pore channels. Different acids (HNO3, H2SO4, H3PO4) were used to catalyze the polymerization reactions to obtain N-doped, S-doped, and P-doped porous carbons, respectively. The adsorption properties of H2, CH4, and CO2 were investigated on these doped carbon materials systematically. For the hydrogen adsorption, the adsorption amount was 11.8%, 21.1%, and 33.3% higher on N-doped, S-doped, and P-doped porous carbons, respectively, than the carbon sample without doping, and the highest hydrogen uptake reached 14.88 mmol g−1 on the P-doped sample; regarding the CO2 adsorption, the adsorption amount reached 3.60 mmol g−1 and 3.16 mmol g−1 on the S-doped sample and N-doped sample, respectively, which is 39.5% and 22.5% higher than the sample without doping; it also shows that methane uptake amount was significantly increased by 27.1% on the S-doped sample as compared to the sample without doping, i.e., 3.52 mmol g−1 of CH4. Therefore, it is predicted that these doped carbon materials with high specific surface area are of great potential for the gas adsorption of H2, CH4, and CO2.
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RSC Advances
·
2015
·Vol. 5
·期 47
·37603-37609
·
IF 3.84
Gui-Sheng Zeng,Jian Yu,Hong-Yun Zhu,Hui-Long Liu,Qiu-Ju Xing,Shao-Kui Bao,Shun He,Jian-Ping Zou,Chak-Tong Au
For the first time, InTaO4 photocatalysts with different morphologies and structures were facilely prepared using a versatile sol precursor. SEM, TEM and HRTEM were used to characterize their structures and morphologies. The as-synthesized materials exhibit different physicochemical properties. Compared to InTaO4 nanoparticles and SiO2@InTaO4 core–shell nanospheres, InTaO4 nanofibers have higher light absorption ability, larger specific surface area, and better photocatalytic activity for hydrogen evolution. We proposed mechanisms for the formation and photocatalytic activity of the three catalysts. The present work not only provides a new approach for the synthesis of tantalates that are different in morphology and structure but also offers new insights into the controllable preparation of photocatalysts through a versatile precursor for environmental and energy applications.
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Advanced Optical Materials
·
2015
·Vol. 3
·期 3
·360-367
·
IF 4.062
Dan Qu,Zaicheng Sun,Min Zheng,Jing Li,Yongqiang Zhang,Guoqiang Zhang,Haifeng Zhao,Xingyuan Liu,Zhigang Xie
A facile solvothermal route to synthesize S,N co-doped graphene quantum dots (S,N-GQDs) with unique optical properties is demonstrated. Three absorption bands are observed at 338, 467, and 557 nm, which is different from any previous reports. The photoluminescent spectra display emissions in three primary colors that are independent of the excitation wavelength, within the excitation wavelength ranges of 340–420 nm, 460–540 nm, and 560–620 nm. The PL excitation spectra indicate that each emission is related to a single excitation band. It is proposed that three independent luminescent centers coexist in S,N-GQDs because the doping with S and N may change the chemical environment of the GQDs. However, energy-transfer processes usually do not occur among the independent luminescent centers under different wavelength light excitation. Heteroatom-doping of GQDs provides an attractive means of effectively tuning their optical properties for the purpose of exploiting new applications in visible-light photocatalytic and bioimaging. S,N-GQDs/TiO 2 composites exhibit better hydrogen production activities under visible light ( λ > 420 nm) than commercial TiO 2 (P25), owing to the presence of characteristic absorption bands in the visible region. Furthermore, the S,N-GQDs have a pronounced biocompatibility and bioimaging ability under long-wavelengths excitation for live A549 cells.
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Journal of Physical Chemistry C
·
2014
·
IF 4.835
Yan Yan,Chao Wang,Xu Yan,Lisong Xiao,Jianghua He,Wei Gu,Weidong Shi
The construction of heterojunction photocatalysts has received much attention in the field of photocatalytic H2 production from water splitting. The surface phase junction of semiconductors is very important to the activity of heterojunction photocatalysts. In this study, an effective anatase–graphene–rutile heterojunction structure was designed and fabricated by using graphene as the surface phase junction between anatase and rutile particles. Results show that both the anatase/rutile ratio (A/R ratio) and graphene amount represent important influence on H2 production activities of anatase–graphene–rutile heterojunction photocatalysts. Under our experimental condition, the optimum A/R ratio is 7/3 and graphene addition amount is 2 wt %, the corresponding AR7/3–2%G sample has the highest H2 production rate of 1.714 mmol/h. By further experimental study, we think the high H2 production activity of anatase–graphene–rutile heterojunction photocatalyst is from the enhanced charge separation rather than other effect. This work values the expanding of surface phase junction and provides a feasible strategy to develop high-performance photocatalysts by designing and expanding the surface phase junction.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Weirong Zhao,Yajun Li,Meng Zhang,Jinsheng Chen,Lihong Xie,Qiaomeng Shi,Xi Zhu
Fe-doped TiO 2 photocatalysts were synthesized rapidly and directly by the microwave–hydrothermal method and evaluated for hydrogen production by water splitting under UV–vis irradiation. The photocatalysts were characterized by X-ray diffraction, transmission electron microscopy, N 2 adsorption–desorption isotherms, inductively coupled plasma atomic emission spectroscopy, UV–vis spectroscopy, X-ray photoelectron spectra and photoelectrochemical experiments. The results showed that Fe-doped TiO 2 photocatalysts synthesized by the microwave–hydrothermal method exhibited a smaller crystallite size and higher specific surface area than TiO 2 photocatalysts. The microwave–hydrothermal method was a feasible way to increase the Fe doping concentration with enhanced electron–hole separation and electron transfer efficiency. It was also observed by first-principles density functional theory calculations that Fe can induce the formation of impurity levels near the valence band, leading to the reduction of the band gap and the improvement of photocatalytic activity. The highest photoactivity was achieved for TiO 2 doped with 0.5% Fe with a hydrogen production rate of 10.95 μmol h −1 .
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Yinghui Zhang,Kun Dong,Meng Zhang,Xiaofei Wang,Xuehong Zhang,Dunqiu Wang,Ruize Sun,Haixiang Li,Wenjie Zhang
Hydrogen-based membrane biofilm reactors using hollow-fiber membrane modules as their functional cores can play an important role in treating oxidizing pollutants. However, most studies have focused on pollutant removal, and few have investigated how membrane material properties affect reactor's operation. Here, we selected polyvinyl chloride (PVC) and polyvinylidene fluoride (PVDF) hollow fiber membrane materials with large differences in membrane surface properties to assemble the reactor, and investigated how the membrane properties affected nitrate removal and EPS secretion in MBfRs. The results showed that the membrane surface zeta potential and membrane contact angle had a certain positive impact on the NO 3 − -N removal rate and total EPS secretion in the MBfRs. When the contact angle (74.51–85.51°) and zeta potential (−12.5–4.5) increased, the biofilm on the membrane surface secreted more binding proteins (90.81–113.54 mg/gVSS), facilitating reactor biofilm growth, pollutant removal, and impact loads. Moreover, the properties of the experimentally selected PVC membrane material are more suitable for MBfR operation and are in line with the fundamental need for energy saving and emission reduction in modern society. This study provides a theoretical basis for the selection of membrane materials to enhance denitrification in H 2 -MBfRs, and an engineering foundation for reactors applications.
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MOLECULES
·
2024
·
IF 4.2
Yuqing Yan,Yonghui Wu,Chenggen Lu,Yu Wei,Jun Wang,Bo Weng,Wei-Ya Huang,Jia-Lin Zhang,Kai Yang,Kangqiang Lu
CdS quantum dots (CdS QDs) are regarded as a promising photocatalyst due to their remarkable response to visible light and suitable placement of conduction bands and valence bands. However, the problem of photocorrosion severely restricts their application. Herein, the CdS QDs-Co 9 S 8 hollow nanotube composite photocatalyst has been successfully prepared by loading Co 9 S 8 nanotubes onto CdS QDs through an electrostatic self-assembly method. The experimental results show that the introduction of Co 9 S 8 cocatalyst can form a stable structure with CdS QDs, and can effectively avoid the photocorrosion of CdS QDs. Compared with blank CdS QDs, the CdS QDs-Co 9 S 8 composite exhibits obviously better photocatalytic hydrogen evolution performance. In particular, CdS QDs loaded with 30% Co 9 S 8 (CdS QDs-30%Co 9 S 8 ) demonstrate the best photocatalytic performance, and the H 2 production rate reaches 9642.7 μmol·g −1 ·h −1 , which is 60.3 times that of the blank CdS QDs. A series of characterizations confirm that the growth of CdS QDs on Co 9 S 8 nanotubes effectively facilitates the separation and migration of photogenerated carriers, thereby improving the photocatalytic hydrogen production properties of the composite. We expect that this work will facilitate the rational design of CdS-based photocatalysts, thereby enabling the development of more low-cost, high-efficiency and high-stability composites for photocatalysis.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2024
·
IF 4.2
Yajie Wang,Yanan Gao,Jingxuan Yang,Bin Liu
C 3 N 5 is emerging as an important visible light catalyst because of its narrow band gap, nontoxicity and thermal stability. Herein, sulfur-doped g-C 3 N 5 (SCN) was prepared by copolymerization of thioacetamide (TAA) and 3-amino-1,2,4-triazole (3-AT). Then copper nanoparticles (Cu NPs) were anchored onto the SCN framework, resulting in the formation of Cu/SCN. It was found that the average H 2 production rate of SCN and Cu/SCN was 0.76 and 1.34 mmol g −1 h −1 , which was much higher than that of C 3 N 5 , respectively. Acting as a new active spots, sulfur doping effectively reduces the band gap of g-C 3 N 5 , and the formation of S-Cu bonds further creates an efficient electron transport pathway. As a result, Cu/SCN possesses a broader visible light absorption spectrum, stronger reduction capability, and greater efficiency in photo-induced carrier separation and transfer. Therefore, this work introduces a novel strategy for design of high efficiency photocatalytic H 2 evolution carbon nitride through non-noble metal and sulfur anchoring junction.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Hongcai Su,Yuheng Wu,Jie Pan,Lingjun Zhu,Shurong Wang,Yanjun Hu
Mixed plastic wastes are posing substantial challenges to the environment due to their mass production and difficulty in separation, especially mixed polyvinyl chloride/polyethylene terephthalate (PVC/PET) plastic wastes. In this work, a novel tandem thermochemical process including hydrothermal depolymerization of mixed PVC/PET plastic wastes, and subsequent catalytic aqueous phase reforming (APR) of hydrolysate solution was developed. The activated carbon derived from PVC (PVC-AC) supported Ru catalysts were prepared and successfully used in the catalytic APR of hydrolysate solution for high-purity H 2 production. Besides, the presence of NaOH realized in-situ capture of CO 2 in APR process, which promoted the water-gas shift reaction and inhibited methanation reactions. As a result, a high H 2 yield of 12.23 mol/kg Plastic with H 2 concentration of ca. 98% was obtained via tandem hydrothermal conversion of mixed PVC/PET plastic wastes. The by-products from the entire tandem process including the terephthalic acid (TPA) and sodium chloride (NaCl) were separated and purified for further industrial application. This work provided a sustainable route for conversion of mixed plastic wastes into value-added fuel.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Gaokui Chen,Qiuwan Shen,Xin Zhang,Tianyun Zhao,Kuanyu Zhu,Shian Li
Methanol steam reforming (MSR) is an effective way to provide high purity hydrogen for PEMFCs, however the main challenge is the toxic effect of CO. In this study, CuGa 2 O 4 spinel catalyst was applied first for MSR at low temperature. The properties of catalysts were characterized by various techniques, the MSR catalytic performance was also studied in deeply. The surface of the catalyst is composed of particle chains that are interconnected, forming high-volume pores that increase the specific surface area. The catalyst also has a rich porous structure, exposing more active sites. Furthermore, the presence of oxygen vacancies facilitates the adsorption of reactive oxygen species, reducing CO generation. A possible pathway for methanol dehydrogenation has been determined using DFT calculations. The relatively low overall energy barrier on the catalyst surface facilitates methanol activation. Among the steps, formaldehyde dehydrogenation is the rate-determining step in the methanol dehydrogenation process. The CuGa 2 O 4 catalyst exhibits good gas selectivity, with a hydrogen selectivity of 98 % and CO selectivity of 0. and no deactivation occurred within 50 h, demonstrating outstanding durability. These features allow it to serve as an efficient catalyst for MSR online hydrogen production and direct supply to PEMFCs.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Gaimei Gao,Mingyu Dou,Xiaojie Liu,Erkang Liu,Zixian Wang,Guang Yang,Hua Yang,Wenning Yang,Dacheng Li,Jianmin Dou
The development of photocatalysts with non-noble metals and the effective separation of photoexcited carriers is a significant strategy for accelerating surface reaction kinetics and promoting water splitting to produce H 2 . Herein, an exquisite core-shell NiFe-LDH@ZnIn 2 S 4 heterojunction photocatalyst was constructed by in situ decoration of ultrathin ZnIn 2 S 4 nanosheets on the surface of the flower-like NiFe-LDH microsphere . The synthesized 3D hierarchical NiFe@ZIS-25 composite exhibits enhanced photocatalytic H 2 evolution activity, reaching 9.12 mmol·h -1 ·g -1 , which is 2.52-fold higher than pure ZnIn 2 S 4 . The significant improvement in H 2 evolution performance could be attributed to the hierarchical core-shell structure of the NiFe@ZIS-25 photocatalyst, which enhanced the light capture ability. In addition, the interfacial coupling effect of ZnIn 2 S 4 and NiFe-LDH is beneficial to the migration of carriers. More importantly, the construction of Z-scheme heterojunction efficiently promotes the fast translation of photogenerated carriers while preserving a stronger reduction potential to achieve H 2 evolution. This work elucidates a rational strategy to develop efficient photocatalysts with hierarchical core-shell structures for water splitting.
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