Journal of Materials Chemistry A
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2018
·Vol. 6
·期 10
·4485-4493
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IF 9.931
Lingyou Zeng,Kaian Sun,Zhichao Yang,Shengli Xie,Yanju Chen,Zhi Liu,Yaqing Liu,Jinchong Zhao,Yunqi Liu,Chenguang Liu
Three-dimensional (3D) nanomaterials have received significant attention for large-scale functional applications due to their large specific surface areas as well as desired electrical, physicochemical, and catalytic properties. Herein, we present a facile and effective synthetic route for in situ grown 3D hierarchical Ni3S2 superstructures (rod-like arrays and nanoforest patterns) on nickel foam. This handy strategy endows the Ni3S2 superstructures with large surface active areas, porosity, and macro-/mesoporous structures. We have shown that these materials can serve as highly active, binder-free, bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Moreover, these materials were found to provide a ∼100% faradaic yield towards both HER and OER and exhibit remarkable catalytic stability (for >50 h).
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2017
·
IF 3.582
Haiyan Shen,Dawei Ni,Ping Niu,Yi Zhou,Tianyou Zhai,Ying Ma
Spatially controlled co-loading of both oxidation and reduction cocatalysts on semiconductor photocatalysts has been demonstrated to be favorable for photogenerated charge separation and thus enhanced photocatalytic activity. Herein, we presented a simple ball-milling method to improve photocatalytic H 2 production of TiO 2 by co-loading of oxidation cocatalyst Co 3 O 4 with reduction cocatalyst CuO , wherein the Co 3 O 4 loading amount was significant especially for TiO 2 loaded with sufficient or optimum CuO. In comparison with that on TiO 2 loaded with only CuO, the photocatalytic H 2 production from water over TiO 2 photocatalyst co-loaded with CuO and trace Co 3 O 4 was enhanced by approximately 5.5 times, even though complex spatial control was not adopted. In contrast, remarkable improvement of photocatalytic activity after Co 3 O 4 co-loading was only observed on TiO 2 photocatalysts loaded with less CuO in the presence of methanol. Better separation of photogenerated charges on the surface of dual-cocatalysts modified TiO 2 was further demonstrated by decreased luminescence as well as increased photogenerated electrons and hydroxyl radicals as compared to those loaded with only CuO.
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Journal of the Taiwan Institute of Chemical Engineers
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2017
·
IF 4.217
Qun-Zeng Huang,Ji-Chao Wang,Li-Qun Ye,Qian Zhang,Hong-Chang Yao,Zhong-Jun Li
The construction of p–n heterojunction is an efficient strategy to restrain photogenerated charge carriers recombination and enhance the photocatalytic efficiency toward H 2 evolution from water splitting. Herein a novel p–n heterojunction Mn 0.25 Cd 0.75 S/Co 3 O 4 was synthesized via facile hydrothermal method. Photocatalytic H 2 evolution of as-synthesized Mn 0.25 Cd 0.75 S/Co 3 O 4 composites in the absence of noble metal co-catalysts under visible light irradiation ( λ ≥ 400 nm) was investigated. The results demonstrated that photocatalytic H 2 evolution of Mn 0.25 Cd 0.75 S was significantly enhanced by loading Co 3 O 4 nanoparticles . It was confirmed that 0.48 wt% of Co 3 O 4 loading content achieved the highest H 2 evolution rate of 25.71 mmol/g/h, which was about 5.35 times higher than that of pure Mn 0.25 Cd 0.75 S. The remarkably improved photocatalytic activity could be attributed to the formation of the p–n junction at the interface between Mn 0.25 Cd 0.75 S and Co 3 O 4 , effectively promoting interfacial charge transfer and separation. This work revealed that the p–n heterojunction Mn 0.25 Cd 0.75 S/Co 3 O 4 may be a promising candidate for efficient energy conversion.
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Inorganic Chemistry Frontiers
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2017
·Vol. 5
·期 2
·370-377
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IF 4.036
Zhujun Zhang,Shiliang Zhang,Qilu Yao,Gang Feng,Meihua Zhu,Zhang-Hui Lu
Metal–organic framework (MOF) immobilized Rh–Ni alloy nanoparticles (NPs) with a mean size of 2.8 nm have been facilely and successfully fabricated via a reduction rate controlled method. Bimetallic NP/MOF composites with uniform tiny RhNi alloy NPs immobilized on MOFs, high surface areas (1970 m2 g−1), and accessible porous structure have been obtained. The resulting RhNi/MOF catalysts show high catalytic activity and robust durability for complete H2 evolution from hydrazine borane (N2H4BH3) and hydrous hydrazine (N2H4·H2O). The optimized Rh0.8Ni0.2/MIL-101 catalyst exhibits excellent catalytic performance for the dehydrogenation of N2H4BH3 and N2H4·H2O in aqueous solution with 100% conversion and hydrogen selectivity, high total turnover frequencies (TOF), up to 1200 and 428.6 mol(H2) mol(Rh+Ni)−1 h−1, respectively, the highest over Rh-based catalysts. The high activity and prominent durability of Rh0.8Ni0.2/MIL-101 are highly dependent on the features of the MOF immobilized tiny RhNi alloy NPs, the strong interaction between the MOF crystal and RhNi alloy NPs, the optimized surface and electronic structure of RhNi alloy with an atomic ratio of 8 : 2, and the accessible open porous structure for free mass transfer.
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APPLIED SURFACE SCIENCE
·
2016
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IF 3.15
Baolin Yan,Juan Zhou,Xiaoyu Liang,Kainan Song,Xintai Su
The production of H 2 by photocatalytic water splitting has become a promising approach for clean, economical, and renewable evolution of H 2 by using solar energy. In spite of tremendous efforts, the present challenge for materials scientists is to build a highly active photocatalytic system with high efficiency and low cost. Here we report a facile method for the preparation of TiO 2 /C nano-flakes, which was used as an efficient visible-light photocatalyst for H 2 evolution. This composite material was prepared by using a phase-transfer strategy combined with salt-template calcination treatment. The results showed that anatase TiO 2 nanoparticles with the diameter of ∼10 nm were uniformly dispersed on the carbon nano-flakes. In addition, the samples prepared at 600 °C (denoted as T600) endowed a larger surface area of 196 m 2 g −1 and higher light absorption, resulting in enhanced photocatalytic activity. Further, the T600 product reached a high H 2 production rate of 57.2 μmol h −1 under visible-light irradiation. This unusual photocatalytic activity arose from the positive synergetic effect between the TiO 2 and carbon in this hybrid catalyst. This work highlights the potential of TiO 2 /C nano-flakes in the field of photocatalytic H 2 evolution under visible-light irradiation.
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CERAMICS INTERNATIONAL
·
2017
·
IF 2.986
Jindou Hu,Yali Cao,Jing Xie,Dianzeng Jia
To reduce the cost of the traditional noble metal-loaded photocatalysts for H 2 production, low-cost Ni(OH) 2 -TiO 2 nanocomposites were designed and synthesized by a simple room-temperature solid-state chemical method (RSCM), which is a facile, low-cost and eco-friendly manipulation. Various testing methods and tools were used to characterize the crystal structure, elemental composition, morphology, light absorption ability, fluorescent performance, photocurrent density, and photocatalytic activity of the obtained nanocomposites. The results indicated that RSCM can be used to synthesize Ni(OH) 2 -TiO 2 nanocomposites with a small size (50 nm) and good dispersity. Compared to pure TiO 2 , the obtained nanocomposites displayed excellent photocatalytic performance for H 2 production by photocatalytic water-splitting. The amount of hydrogen needed for the optional nanocomposite NOT-1 was 9180 μmol/g, which is 29 times that of the commercial P25. The reason for the improved performance for photocatalytic hydrogen production is that the existing Ni(OH) 2 in nanocomposites promoted the separation between the photogenerated electron and holes.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2016
·Vol. 24
·期 1
·676-684
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IF 2.76
Tu Baosheng,Shi Nian,Sun Wei,Cao Limei,Yang Ji
In this paper, Pt supports on carbon black powder (Vulcan XC-72) were synthesized via a hydrothermal method for selective catalytic reduction (SCR) of NO with H 2 in the presence of 2 vol% O 2 over a wide temperature of 20–300 °C. The results showed that the 3 and 5 wt% Pt/C catalysts resulted in high NO conversion (>90 %) over a temperature range of 120 to 300 °C, and the maximum NO conversion of 98.6 % was achieved over 5 wt% Pt/C at 120 °C. Meanwhile, the influence of SO 2 and H 2 O on the catalyst performance of 3 wt% Pt/C was investigated. The catalysts exhibited good SO 2 poisoning resistance when the SO 2 concentration was lower than 260 ppm. Moreover, a positive effect on NO conversion was detected with the addition of 3 and 5 vol% H 2 O in the feed gas stream.
TEM image and good NO conversion performance of the Pt/C catalysts
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Journal of Energy Chemistry
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2017
·
IF 2.594
Ya'nan Yao,Yan Gao,Lu Ye,Hu Chen,Licheng Sun
The development of efficient molecular catalysts for visible-light driven CO 2 reduction, based on abundant materials, is necessary to meet energy demands and address environment problems. In this work, a Co(bpy) 2 Cl 2 catalyst was developed and showed high efficiency and durability for the photocatalytic reduction of CO 2 and protons. Yields of CO and H 2 as high as 62.3 and 69.9 µmol were achieved and the turnover numbers (TONs) reached 6230 and 6990, respectively, under light irradiation ( λ > 420 nm) for 4 h, indicating that the mixture gases could be a candidate as syngas . The apparent quantum yield was determined to be 2.1% for CO. Mechanistic studies revealed oxidative quenching of the photosensitizer Ru(bpy) 3 Cl 2 by the catalyst. The photocatalytic performance, flexible synthesis and non-noble metal catalyst in our system show great promise for the practical application of Co(bpy) 2 Cl 2 to photocatalytic reduction of CO 2 .
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Qian Yu,Bilin Liang,Siqi Jia,Fang Li,Qiming Li
A novel approach was developed to fabricate defect-free MIL-96 membranes on an α-Al 2 O 3 support by combining aluminum isopropoxide coating with mixed-solvent regulation. The aluminum isopropoxide gel on the support functions as an active Al source, directing MIL-96 crystal nucleation and growth. A subsequent secondary crystallization can produce a well-intergrown MIL-96 membrane. Here, the gel coating inhibits the preferential crystallization of MIL-96 particles in the support pores, optimizing the microstructure and diminishing inter-crystal defects. By accurately adjusting the formic acid to N-methylformamide ratio in synthesis solution, a balance between membrane crystallinity and formation is achieved. Membrane separation property evaluation revealed an outstanding H 2 permeance of 1800 GPU and an H 2 /CO 2 separation factor of over 24.0, outperforming some advanced polycrystalline MOF membranes. This approach provides a potentially cost-efficient method for the large-scale preparation of MIL-96 membranes, holding great potential for practical applications in membrane separation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Lei Zhang,Zhiyuan Jiang,Jingru Guo,Chao Zhang,Xiaolong Xu,Dong Shi,Yongliang Shao,Zizheng Ai,Yongzhong Wu,Xiaopeng Hao
An in-depth understanding of structure-activity relationship between the phase constitution and solar-to-hydrogen (STH) conversion efficiency is conducive to guiding the optimization route of targeted photocatalyst candidates, further establishing advanced photocatalytic systems. Herein, based on the concept of phase engineering, we encompassed the crystalline phase of CdS and achieved precise regulation of phase proportion as well as phase boundary width in the phase junction for the first time. The above cooperative effect not only modifies energy band distribution for sufficient redox potentials, but also guarantees the reverse migration orientation of photogenerated carriers in phase junction, thereby endowing photocarriers with a prolonged lifetime. Compared to pure cubic or hexagonal phase (72.6 or 101.1 μmol h −1 g −1 ), this CdS system with optimized phase junction demonstrates an improved photocatalytic hydrogen evolution activity of 1.04 mmol h −1 g −1 and favorable stability without cocatalyst assistance, which mainly stems from an efficient protons reduction process interacting with long-lived photogenerated electrons. This research explores the mechanism behind phase regulation and its relationship with junction capability, providing a powerful strategy to manipulate crystal phase distribution and paving a feasible avenue for other phase-dependent photocatalysts towards rational design of heterostructures based on different phases in solar energy conversion field.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
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IF 14.7
Wan Sijie,Wang Wang,Cheng Bei,Luo Guoqiang,Shen Qiang,Yu Jiaguo,Zhang Jianjun,Cao Shaowen,Zhang Lianmeng
The rapid recombination of photoinduced charge carriers in semiconductors fundamentally limits their application in photocatalysis. Herein, we report that a superlattice interface and S-scheme heterojunction based on Mn 0.5 Cd 0.5 S nanorods can significantly promote ultrafast charge separation and transfer. Specifically, the axially distributed zinc blende/wurtzite superlattice interfaces in Mn 0.5 Cd 0.5 S nanorods can redistribute photoinduced charge carriers more effectively when boosted by homogeneous internal electric fields and promotes bulk separation. Accordingly, S-scheme heterojunctions between the Mn 0.5 Cd 0.5 S nanorods and MnWO 4 nanoparticles can further accelerate the surface separation of charge carriers via a heterogeneous internal electric field. Subsequent capture of the photoelectrons by adsorbed H 2 O is as fast as several picoseconds which results in a photocatalytic H 2 evolution rate of 54.4 mmol·g −1 ·h −1 without any cocatalyst under simulated solar irradiation. The yields are increased by a factor of ~5 times relative to control samples and an apparent quantum efficiency of 63.1% at 420 nm is measured. This work provides a protocol for designing synergistic interface structure for efficient photocatalysis.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Chuanhao Li,Yi Tian,Shuangyu Wang,Ping Yang,Xiao Zhang
To improve the stability of Ag based co-catalysts and to increase the photocatalytic performance of graphitic carbon nitride (g-C 3 N 4 ), Ag 2 Se nanoparticles were grown onto superior thin sulfur-doped g-C 3 N 4 nanosheets which was fabricated via two-step thermal polymerization at high temperature. Ultrathin S-doped g-C 3 N 4 nanosheets were prepared via two-step thermal polymerization using melamine and thiourea. The ratios of Ag 2 Se were adjusted to fabricate a series of Ag 2 Se/S-g-C 3 N 4 (Ag 2 Se/SCN) composite samples by controlled solvothermal synthesis. S-doping plays an important role in mono-dispersion of Ag 2 Se nanoparticles on S-g-C 3 N 4 nanosheets because of the control of growth sites. The photocatalytic removal of tetracycline hydrochloride test indicates that sample Ag 2 Se/SCN-3 with Ag 2 Se loading of 3 % reveals the best removal effect, in which tetracycline hydrochloride of 60 % is removed within 60 min. Photocatalytic hydrogen generation test results without co-catalyst addition demonstrate that sample Ag 2 Se/SCN-3 exhibits the best H 2 evolution rate of 2116.35 μmol·g −1 ·h −1 , which is 3.8 times of that of pure carbon nitride. The photocatalytic mechanism tests suggest that Schottky heterojunctions are formed in the Ag 2 Se/S-g-C 3 N 4 composites. The formation of Schottky heterojunctions improved the separation efficiency of photogenerated charge carriers. The incorporation of Ag 2 Se nanoparticles (as the co-catalyst) on S-g-C 3 N 4 nanosheets is the key for drastically improving the photocatalytic performance and eliminating the use of Pt co-catalyst during the photocatalytic processes.
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