FUEL
·
2018
·
IF 4.908
Yaqiu Tao,Lulu Tao,Zhigang Pan,Simin Qiu,Xiaodong Shen
Formic acid is a promising hydrogen storage material for its high H 2 capacity, easy transfer and moderate H 2 regeneration conditions. Active carbon supported Mo 2 C with or without Co doping were used as the heterogeneous catalyst in the decomposition of a high concentrated aqueous solution of formic acid up to 50% on a fixed bed reactor. For a given flow rate and reaction temperature, though higher volume of H 2 is produced per unit time, the increase in formic acid’s concentration reduces both H 2 selectivity and formic acid conversion rate. At 250 °C, a stream of 236 mL/min H 2 was generated continuously at a high H 2 selectivity (91%) and formic acid conversion rate (86%), from a 10% formic acid fed at the flow rate of 5 mL/min. High reaction temperature improved the conversion of formic acid feed at little expense of H 2 selectivity. The doping of Co in the Mo 2 C lattice improves the H 2 selectivity to 100% at 100–200 °C. A life time study showed the stability of this system by the remained high H 2 selectivity in formic acid decomposition. This work of using active carbon supported molybdenum carbides and high concentrated aqueous formic acid, opens up a new route for the portable H 2 generator using formic acid as a hydrogen storage material at no environmental risk.
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高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 33
·11705-11712
·
IF 4.099
Cong-Cong Shen,Ya-Nan Liu,Xin Wang,Xiao-Xiang Fang,Zhi-Wei Zhao,Nan Jiang,Liu-Bo Ma,Xiao Zhou,Tuck-Yun Cheang,An-Wu Xu
Metal–organic framework (MOF)-based materials possess numerous attractive characteristics; however, the application of MOF-based photocatalysts in the area of visible-light photocatalytic H2 evolution is still in its infancy. Herein, we develop a series of novel UiO-66-NH2-based composites with embedded NiO nanoparticles via solvothermal treatment and subsequent calcination. Their characterizations demonstrate intimate lattice-level contacts between UiO-66-NH2 photocatalysts and NiO nanoparticles. By optimizing each component, even without noble metal loading, the U6N-NiO-2 sample (the weight ratio of NiO to U6N-NiO-2 is theoretically calculated to be ca. 10 wt%) with 15 mg eosin Y as a sensitizer causes an enhanced H2 generation rate of 2561.32 μmol h−1 g−1 under visible-light irradiation using TEOA as a sacrificial reagent; furthermore, its corresponding quantum efficiency is as high as 6.4% at 420 nm. The H2 evolution activity of U6N-NiO-2 is about 5 times higher than that of the UiO-66-NH2 photocatalyst (denoted as U6N) and 23 times higher than that of U6N-NiO-2 without sensitizer. It is demonstrated that the high efficiency originates from the visible-light generated electrons of eosin Y and UiO-66-NH2, the efficient separation of carriers by the cascaded band structure and more negative CB of NiO as well as the good dispersion of NiO nanoparticles on the octahedral skeleton. This study provides new insights for the design of MOF-based materials without noble metal loading for visible-light photocatalytic H2 evolution.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Qun-Zeng Huang,Ze-Juan Tao,Li-Qun Ye,Hong-Chang Yao,Zhong-Jun Li
Development of highly efficient and low-cost noble metal-free co-catalysts for photocatalytic H 2 evolution from water splitting has been aiming at a long-term goal of a renewable hydrogen economy. Herein, a series of novel Mn 0.2 Cd 0.8 S/CoP 3 composites have been successfully prepared through loading CoP 3 nanoparticles on the surface of one dimensional (1D) Mn 0.2 Cd 0.8 S nanowires (NWs) by a facile solvothermal method. Under visible light (λ ≥ 420 nm) irradiation, the as-prepared Mn 0.2 Cd 0.8 S/CoP 3 composite with 2.87 wt% of CoP 3 displayed the highest photocatalytic H 2 evolution activity with a corresponding H 2 evolution rate of 29.53 mmol g −1 h −1 and an apparent quantum yield of 29.2% at 420 nm, which was about 5.02 times higher than that of pure Mn 0.2 Cd 0.8 S and 1.79 times than that of Mn 0.2 Cd 0.8 S/Pt-1.5 wt%. Moreover, the Mn 0.2 Cd 0.8 S/CoP 3 composite exhibited excellent photostability. The superior photocatalytic activity of Mn 0.2 Cd 0.8 S/CoP 3 composite was predominantly attributed to the synergistic effects of highly efficient charge separation efficiency and sufficient active sites for H 2 evolution reaction. This work revealed that low-cost CoP 3 can replace noble metal Pt as a highly efficient co-catalyst for enhancing the photocatalytic activity of semiconductor materials.
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高影响因子
Catalysts
·
2019
·Vol. 9
·期 7
·616
·
IF 3.444
Ruizhou Gan,Xiaohua Ma,Guorong Wang,Zhiliang Jin
CoSe2,as a kind of co-catalyst, would replace noble metals element to dope pure CdS. The CoSe2/CdS photocatalyst could be synthesized by simple physical mixing. With the introduction of CoSe2, especially 30% CoSe2/CdS, hydrogen production would be about 500 μmol within 5 h, five times that of pure CdS under the same conditions. The CoSe2/CdS photocatalyst could bear four cycles of hydrogen evolution and sustain the hydrogen production, with a minor decrease. In other words, the electron transition velocity would surge along with the introduction of CoSe2particles. The CoSe2could be deemed as the predator and exit of electrons to inspire the detachment of the hole-electron pairs and relieve the recombination of the hole-electron pairs.Keywords:CoSe2clusters;CdS nanorod;hydrogen evolution;photocatalysis
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2012
·
IF 5.625
Ting Bao,Zhongkui Zhao,Yitao Dai,Xiaoli Lin,Ronghua Jin,Guiru Wang,Turghun Muhammad
CO preferential oxidation (PROX) reactions were performed over the supported Co 3 O 4 -CeO 2 catalysts on modified activated carbon (AC) for eliminating the trace CO from H 2 -rich gases. The effects of support modification by H 2 O 2 oxidation treatment , catalyst calcination temperature, Ce/Co atomic ratio ( n Ce/Co ), Co 3 O 4 -CeO 2 loading and reaction parameters on catalytic properties of the Co 3 O 4 -CeO 2 /AC catalysts were investigated. Various characterization techniques like scanning electron microscopy (SEM), X-ray diffraction (XRD) and H 2 temperature-programmed reduction (H 2 -TPR) were employed to reveal the relationship between catalysts nature and catalytic performance. Results illustrate that the supported Co 3 O 4 -CeO 2 catalyst on modified AC exhibits excellent catalytic properties, which highly depends on dispersity and reducibility of Co 3 O 4 affected by the time of support treatment ( t p ), calcination temperature, n Ce/Co and loading. The supported 35 wt% Co 3 O 4 -CeO 2 catalyst (1:8 of n Ce/Co ) on the modified AC with H 2 O 2 oxidation treatment for 6 h demonstrates the best catalytic properties and the almost complete CO transformation takes place in a wide temperature range of 125–190 °C. Moreover, it is also found that the developed catalyst exhibits an outstanding catalytic stability, and 100% CO conversion can be maintained as the time on stream evolutes up to 1800 min even in the presence of CO 2 and H 2 O in the feed. The optimized Co 3 O 4 -CeO 2 /AC may be a robust and promising catalyst for eliminating trace CO from H 2 -rich gases.
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Green Energy & Environment
·
2024
·
IF 10.7
Yi-lei Li,Xu-jia Liu,Yun-biao Wang,Ying Liu,Rui-hong Liu,Hui-ying Mu,Ying-juan Hao,Xiao-jing Wang,Fa-tang Li
Adjusting the interfacial transport efficiency of photogenerated electrons and the free energy of hydrogen adsorption through interface engineering is an effective means of improving the photocatalytic activity of semiconductor photocatalysts. Herein, hollow ZnS/NiS nanocages with ohmic contacts containing Zn vacancy (V Zn -ZnS/NiS) are synthesized using ZIF-8 as templates. An internal electric field is constructed by Fermi level flattening to form ohmic contacts, which increase donor density and accelerate electron transport at the V Zn- ZnS/NiS interface. The experimental and DFT results show that the tight interface and V Zn can rearrange electrons, resulting in a higher charge density at the interface, and optimizing the Gibbs free energy of hydrogen adsorption. The optimal hydrogen production activity of V Zn -ZnS/NiS is 10,636 μmol h −1 g −1 , which is 31.9 times that of V Zn -ZnS. This study provides an idea for constructing sulfide heterojunctions with ohmic contacts and defects to achieve efficient photocatalytic hydrogen production.
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高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
RongQin Ye,HuaBin Fang,Yan-Zhen Zheng,Nan Li,Yuan Wang,Xia Tao
A novel direct Z-scheme CoTiO3/g-C3N4 (CT-U) photocatalytic system with different weight percentage of CoTiO3 was synthesized using a facile in situ growth method for H2 evolution from water splitting. The as-prepared CT-U composites composed of 1D CoTiO3 microrod and 2D g-C3N4 nanosheet were characterized by various techniques including XRD, SEM, TEM, XPS, FTIR, and UV–vis. Results demonstrate that the CT-U composite photocatalysts were successfully fabricated, with intimate interfacial contact and heterojunction interaction between g-C3N4 and CoTiO3 which can significantly boost the photocatalytic activity compared with prinstine g-C3N4 and CoTiO3. The most enhanced H2-evolution rate of 858 μmol h–1 g–1 and high quantum efficiency (38.4% at 365 nm, 3.23% at 420 ± 20 nm) are achieved at an optimal 0.15% CT-U. Meanwhile, the 0.15% CT-U sample exhibits good photocatalytic stability in recycling H2 evolution. Accordingly, direct Z-scheme mechanism capable of leading efficient charge carrier separation and strong reduction ability for enhanced H2 production was proposed, and further evidenced by PL, photoelectrochemical analysis, and ESR assay.
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PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 67
·54769-54776
·
IF 3.84
Chunxiao Lu,Yang Chen,Yun Li,Chunhong Ma,Hongbo Zhang,Yuwei Guo,Jun Wang
A highly effective and stable up-conversion luminescence agent, Er3+:Y3Al5O12, was synthesized by sol–gel and calcination methods. Then, as a novel visible-light photocatalyst, Er3+:Y3Al5O12, Pt and PdS (as dual co-catalysts) decorated ZnS nano-sized composites, Er3+:Y3Al5O12/Pt–PdS/ZnS, were fabricated by deposition–precipitation and ultrasonic dispersion methods. All prepared samples were characterized by X-ray diffractometry (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDX). UV-vis absorption and PL spectra of Er3+:Y3Al5O12 were also determined. The visible-light photocatalytic H2 production activity of the prepared Er3+:Y3Al5O12/Pt–PdS/ZnS was evaluated by using Na2S and Na2SO3 as sacrificial reagents in an aqueous solution under 300 W irradiation from a xenon lamp. In addition, some influential factors such as Er3+:Y3Al5O12 and ZnS mass ratio, catalyst amount, irradiation time and irradiation intensity on visible-light photocatalytic H2 production of Er3+:Y3Al5O12/Pt–PdS/ZnS were investigated in detail. It was found that Er3+:Y3Al5O12 can effectively improve the visible-light photocatalytic activity of ZnS. Particularly, Er3+:Y3Al5O12/Pt–PdS/ZnS with 0.13 wt% PdS and 0.3 wt% Pt and a 0.30 : 1.00 mass ratio shows the highest photocatalytic H2 production activity in the sulfide/sulfite (0.2 mol L−1 Na2S and 0.3 mol L−1 Na2SO3) aqueous solution as sacrificial reagents.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2014
·
IF 2.93
Junxian Wang,Jie Huang,Haolong Xie,Ailan Qu
A photocatalyst composed of graphite-like carbon nitride (g-C 3 N 4 ) and TiO 2 was fabricated by a simple method to calcine the mixture of melamine and TiO 2 precursor. The photocatalyst has enhanced photoactivity for hydrogen evolution from water. Characterization by XRD , FTIR, SEM and elemental analysis showed that the crystal structure and morphologies of composites were affected by the amount of melamine in the composite. The UV–Vis characterization displayed that the optical absorption range of g-C 3 N 4 /TiO 2 hybrid was broadened with a synergistic effect . The photoactivity for H 2 evolution was shown that the best result obtained from the composite with 67 wt% melamine has about 5 times improvement compared with bare TiO 2 or pure g-C 3 N 4 . The enhanced photoactivity might be related with the favorable structure resulted from heat-treatment temperature, and the content of g-C 3 N 4 participating in wide optical absorption, separation and transportation of electronic-holes, as well as morphology of composite.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2014
·
IF 2.93
Jian Yu,Si-Liang Lei,Tong-Cai Chen,Jian Lan,Jian-Ping Zou,Lin-Hua Xin,Sheng-Lian Luo,Chak-Tong Au
A new strategy has been put forward to improve the performance of photocatalytic H 2 evolution of tantalate-based catalysts through designing solid solutions Bi 1− x In x TaO 4 combined with CdS, among which the solid solutions Bi 1− x In x TaO 4 ( x = 0, 0.1, 0.3, 0.5, 0.7, 0.9, and 1.0) were firstly synthesized by the citrate method using cheap and environment-friendly Ta 2 O 5 . The experimental results reveal that the Bi 0.5 In 0.5 TaO 4 solid solution shows the best photocatalytic performance among the Bi 1− x In x TaO 4 solid solutions. And in the absence of noble metals, the 30% CdS/Bi 0.5 In 0.5 TaO 4 (30CBITO) catalyst exhibits good photocatalytic hydrogen evolution from water splitting with a rate of H 2 production of 511.75 μmol h −1 g −1 under simulated sunlight irradiation. And the rate of hydrogen evolution does not markedly change for 60 h. Their compositions , structures and morphologies were characterized by UV–vis diffusion reflectance spectroscopy (DRS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and high resolution transmission electron microscopy (HRTEM). A photocatalytic enhancement mechanism was put forward to elucidate the superior photocatalytic activity and long-term stability of the heterostructured CdS/Bi 0.5 In 0.5 TaO 4 composites.
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高影响因子
Journal of Physical Chemistry C
·
2015
·
IF 4.772
Yunfang Ji,Wei Guo,Huihui Chen,Longshuai Zhang,Song Chen,Mutian Hua,Yuhan Long,Zhuo Chen
Constructing unique nanocomposites to facilitate charge transfer and promote catalytic activity provides a promising approach for enhancing solar-to-hydrogen efficiency. However, revealing the catalytic surface state and understanding their roles in the photocatalytic process remain elusive. Here, we develop a facile and mild solution method for ultrathin TiO2 nanosheets with a large specific surface area and enhanced surface Ti3+ accumulation. Moreover, we demonstrate a hybrid nanosystem composed of ultrathin 2D TiO2 nanosheets directly coupled with 0D CdSe QDs for hydrogen generation. The 0D CdSe QDs increase visible light absorption ability after being coupled with the TiO2 nanosheets. Owing to the synergistic effect between the quantum dots and nanosheets, the apparent quantum efficiency increases to 45% at 380 and 450 nm, and the H2 evolution exhibits a 10-fold enhancement. EPR results indicate that the surface Ti3+ greatly promotes H free radical production due to the redox couple Ti3+/Ti4+ providing an efficient route for the photoexcited electron–hole separation. Our findings provide new insights toward understanding and exploiting highly efficient photocatalyst.
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高影响因子
Sustainability
·
2024
·Vol. 16
·期 10
·4231
·
IF 3.3
Ke Ren,Fangjie Ding,Lijun Zhang,Fengping Peng,Jianzhong Guo,Chunzheng Wu
The food industry is responsible for generating considerable amounts of waste, such as excess fruits and leftover sugars, which contribute to resource depletion and pose environmental challenges. This research delves into the application of gold-modified graphitic carbon nitride nanosheets (Au/CN) as a potent catalyst for the transformation of these food wastes into H2via piezoelectric reforming during sonication. Au/CN demonstrated a superior rate of H2evolution compared to pristine g-C3N4(i.e., 1533.3 vs. 364.9 µmol/g/h) and it maintained its efficiency through multiple cycles of use. The catalytic activity was found to be optimal at a neutral pH level and with increased sugar concentrations. The enhanced catalytic performance of Au/CN was ascribed to the efficient segregation of charge carriers as well as the reduced charge transfer distance. This study underscores the viability of using Au/CN as a means for converting food wastes into a sustainable source of H2energy.
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