INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Keke Dong,Han Li,Chengjia Zhang,Man Zhou,Qian Liang,Yanan Wang,Zhongyu Li,Song Xu
Improving the stability and electron-hole separation efficiency of semiconductor photocatalysts has always been a hot topic in the field of catalysis. In the present study, a novel Cu 2-x S@Mn 0.3 Cd 0.7 S (Cu 2-x S@MCS) core-shell heterojunction has been constructed by the in-situ traditional hydrothermal reaction on the basis of hollow Cu 2-x S nanocubes. The optimized Cu 2-x S@MCS-2 photocatalyst with expanded light absorption exhibits excellent stability and a higher hydrogen evolution rate of 42.43 mmol g −1 h −1 , which is 2.3 times and more than 1400 times contrasting to the pure Mn 0.3 Cd 0.7 S and Cu 2-x S, respectively. Multiple characterizations and structure analysis revealed that the Cu 2-x S@MCS heterojunction possesses outstanding charge separation efficiency and a wider specific surface area which can provide abundant active sites. Furthermore, the mechanism of photocatalytic H 2 evolution for Cu 2-x S@Mn 0.3 Cd 0.7 S S-scheme heterojunction is also proposed. This work thus provides a favorable strategy to inhibit the photogenerated charge carrier recombination and drive highly efficient photocatalytic hydrogen generation by synthesizing photocatalyst with in situ core-shell structures.
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ACS Applied Energy Materials
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2023
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IF 6.4
Yuqing Hu,Puhui Deng,Wenying Wang,Linping Zhang,Yu Hou
Element doping and collaboration with other cocatalysts are two vital strategies to improve the photoelectrochemical properties and overcome the drawbacks of CdS for better photocatalytic performance. In this work, a series of manganese cadmium sulfides (MnxCd1–xS) were obtained by a solvothermal method. When x is equal to or greater than 0.3, MnxCd1–xS is composed of Mn–Cd–S sosoloid and MnS. Among all these MnxCd1–xS products, the Mn0.5Cd0.5S sample showed the best photocatalytic hydrogen production (5.99 mmol g–1 h–1). To further elevate the hydrogen production rate of Mn0.5Cd0.5S, four kinds of Ni-POMs were coupled with it as cocatalysts, and all these composite photocatalysts displayed enhanced performance. The highest efficiency was observed for 15-Ni4–Mn0.5Cd0.5S, which is up to 36.58 mmol g–1 h–1. Various characterizations indicated that Ni4P2W18, Mn–Cd–S sosoloid and MnS in the 15-Ni4–Mn0.5Cd0.5S composite form a double type-II heterojunction, which facilitates the separation and transfer of photogenerated carriers.
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MACROMOLECULAR RAPID COMMUNICATIONS
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2023
·Vol. 44
·期 24
·2300477
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IF 4.6
Yuan Liu,Binghui Xue,Jiadong Chen,Yuyan Lai,Panchao Yin
The emergence of polymers with intrinsic microporosity provides solutions for flexible gas separation membranes with both high gas permeability and selectivity. However, their applications are significantly hindered by the costly synthetic efforts, limited availability of chemical systems, and narrow window of microporosity sizes. Herein, flexible mixed matrix membranes with tunable intrinsic microporosity can be facilely fabricated from the coordination assembly of polymer brushes and coordination nanocages. Polymer brushes bearing isophthalic acid side groups can coordinate with Cu 2+ to assemble into polymer networks crosslinked by 2 nm nanocages. The semi-flexible feature of the polymer brush and the high crosslinking density of the network prevent the network from collapsing during solvent removal and the obtained aerogels demonstrate hierarchical structure with dual porosity from the crosslinked polymer network and coordination nanocage, respectively. The porosity can be facilely tuned via the amount of Cu 2+ by regulating the network crosslinking density and nanocage loadings, and finally, optimized gas separation that surpasses Robeson upper bound for H 2 /CO 2 can be achieved. The coordination-driven assembly protocol paves a new avenue for the cost-effective synthesis of polymers with intrinsic microporosity and the fabrication of flexible gas separation membranes.
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Journal of the Taiwan Institute of Chemical Engineers
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2023
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IF 5.7
Linjuan Wang,Mingpu Kou,Julie Tournet,Siva Karuturi,Ling Zan
Background Recognized for its high calorific value, clean and non-polluting properties, hydrogen is considered to be one of the most attractive solutions to the impending energy crisis. Photocatalytic water splitting has been widely investigated for its promise to produce hydrogen in a sustainable, environmentally friendly and low-cost approach. In pursuit of high photocatalytic efficiency, multiple strategies haven been explored such as doping, co-catalyst modification and heterojunction construction realizing promising improvements. Methods We synthesized CdS doped with Zn ions and modified with MoS 2 as co-catalyst to form Zn x Cd 1− x S solid solution and MoS 2 -Zn 0.25 Cd 0.75 S heterojunction using a simple one-step hydrothermal method. The synthesized catalyst was used water splitting under visible light irradiation. The structural and morphological characteristics of these materials, along with their photocatalytic mechanisms, were investigated using multiple techniques such as SEM, TEM, XPS, PL, etc. Findings The photocatalyst consisting of 0.9 wt.% MoS 2 -Zn 0.25 Cd 0.75 S achieved a production rate of 6276 μmol h −1 g −1 , which is 17.4 times higher than that of pure CdS and 1.6 times higher than that of Zn 0.25 Cd 0.75 S. The composite also demonstrated a high apparent quantum yield of 11.1 % at 420 nm. The mechanism of the water splitting process, revealed through various techniques, introduces novel pathways for crafting high-efficiency photocatalysts with an internal electron-hole separation heterostructure.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Zhiwei Dong,Yudong Ding,Fei Chen,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
The inefficient conversion of carbon dioxide (CO 2 ) to methane often restricts the advancement of CO 2 biomethanation technologies . This study explored the degrading performance, microbial community compositions, and functional gene abundance to examine the impact of zirconium metal-organic frameworks (Zr-MOFs) on the CO 2 biomethanation process. The results showed that the maximum utilization rates of CO 2 and H 2 increased by 2.77 times and 2.36 times after the addition of Zr-MOFs, respectively, and the corresponding conversion rate of CO 2 to methane also increased by 57.53%. Additionally, Zr-MOFs enhanced the COD removal efficiency and hydrolysis of tryptophan-like proteins and humic acid-like substances, resulting in more volatile organic compounds, such as tetradecane, 2-pentanone, and hexadecanoic acid. The analysis of microbial community structure revealed that the relative abundance of Methanothrix and Metanobacterium increased by 24.40% and 36.02% after the addition of Zr-MOFs, respectively. The methane metabolism revealed that Metanobacterium was a member of the same aceticlastic methanogenic pathway as Metanothrix , which encodes acetyl-CoA synthetase to catalyze the synthesis of acetyl-CoA from acetate, and Zr-MOFs also increased the relative abundance of genes that encode the enzyme responsible for converting intermediates to methane. Finally, Zr-MOFs improved the biogenesis and utilization of acetate and hydrogen (H 2 ) by enhancing the activity of enzymes, thereby providing more nutrients for methanogenesis . This study provided thorough explanations for the application and improvement of Zr-MOFs in CO 2 biomethanation technology.
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ACS Applied Nano Materials
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2021
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IF 5.097
Chao Gai,Xia Wang,Jinghai Liu,Zhengang Liu,Yong Sik Ok,Wen Liu,Alex C. K. Yip
Aqueous-phase reforming of organic molecules to hydrogen is a promising strategy to address the production and storage of sustainable hydrogen with lower costs; however, the synthesis of inexpensive transition metal (TM) catalysts with desirable activity and stability for the reaction is still challenging. In this work, a green and efficient approach for modulating the geometric/electronic structure of metal/hydrochar nanocomposites from sustainable biomass was proposed for enhancing H2 production via aqueous-phase reforming of methanol (APRM). A Ni/HC nanocomposite with a special thistle (a perennial species of flowering plant)-like three-dimensional (3D) architecture was first constructed as a model catalyst to expatiate the critical role of modulating an ordered mesoporous structure and interface electron transfer for enhancing APRM. Deliberately balancing heteroatom doping and soft templates contribute to the successful fabrication of the thistle-like superstructure, and such hierarchically porous architectures demonstrated efficient catalysis for APRM, owing to their unique properties, including a highly uniform morphology, narrow particle size distribution, and mesoporous texture with excellent accessibility. In addition, the experimental investigation and density functional theory calculations both substantiated that the combination of heteroatom doping and soft templates was beneficial for the strong electronic metal–support interaction (EMSI) of the metal/hydrochar nanocomposite, which leads to enhanced methanol adsorption, activation, and subsequently improved APRM performance. The electronic structure of the metal/hydrochar nanocomposite played a more significant effect on the intrinsic APRM activity than the geometric structure like the formation of the thistle-like superstructure. Benefiting from the tailored electronic and geometric structure, the resulting Ni0.1/HC-N1.5-S1 catalyst exhibited an unprecedented average turnover frequency (TOF) of 89.5 molH2/molNi/min, higher than any other known platinum group metal-free catalysts, approaching the reactivity of the state-of-the-art noble metal-based APRM catalysts, while showing excellent stability over 10 consecutive reaction cycles.
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FUEL
·
2021
·
IF 6.609
Xianyao Yan,Yingjie Li,Chunxiao Zhang,Yuzhuo Wang,Jianli Zhao,Zeyan Wang
The water gas shift reaction is an important reaction for H 2 production in various industrial applications. The presence of CaO can promote the reactivity of the water gas shift reaction without any catalysts, but the enhancement mechanism of CaO in this reaction is difficult to determine just by the experiment. In this work, the water gas shift reaction along four possible pathways on the CaO surface were studied by density functional theory (DFT) analysis. The energy barriers along the pathways were analyzed to determine the most possible reaction pathway and role of the CaO surface. The DFT calculation results show that the WGS reaction is more prone to proceed along the redox-a pathway probably: H 2 O dissociates into hydroxyl and atomic H spontaneously when H 2 O and CO co-adsorb on the CaO surface, then the hydroxyl continues to dissociate and CO is oxidized by the generated atomic O. Afterwards, H 2 molecule generates from two atomic H, and then CO 2 adsorbs and H 2 desorbs simultaneously on the CaO surface. The CaO surface enables the spontaneous dissociation of H 2 O, which is the rate-limiting step of WGS reaction. The generation of CO 2 is facilitated, and the energy barrier is reduced from 2.304 to 0.757 eV on the CaO surface. Besides, the formation of CO 3 2− on the surface avoids the energy barrier for CO 2 desorption, while the CO 2 also occupies the active site and reduces the enhancement of CaO on WGS reaction. The calculation result reinforces the comprehension on the mechanism of CaO on WGS reaction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Munir Ahmad,Xie Quan,Shuo Chen,Hongtao Yu,Zhenxing Zeng
Metal sulfide photocatalysts have been leading edge for hydrogen evolution reaction (HER) and solar energy conversion due to their suitable electronic and optical properties. The efficiency of these photocatalysts is mostly restricted by slow transfer of photogenerated holes and sluggish water dissociation kinetics. Here, we proposed HER catalyst comprising of Pt-CrO x sites loaded on ZnCdS nanocrystal (ZnCdS/Pt-CrO x ) that employing a redox couple ( OH/OH − ) transport mechanism to efficiently relay of holes in alkaline media. The Pt sites provide optimal hydrogen adsorption energy and CrO x sites support water dissociation, which speed up water dissociation kinetics and leads to a noticeable enhance in HER (21.1 mmol g −1 h −1 ) and phenol degradation. Such efficient activity could be associated to a better mobility of redox couple and fast water dissociation kinetics in alkaline solution. These types of related works open pathways to generate hydrogen from the sea water, largest water source on earth.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Ge Yang,Hailing Guo,Zixi Kang,Shou Feng,Lei Zhao,Svetlana Mintova
Sandwich-type membranes comprising of graphene oxide (GO) as a “bun” and sodalite (SOD) nanocrystals with different morphologies and sizes as an inner layer were prepared. First, the SOD nanocrystals with spheroidal (size of 30 nm) and flake-like (size of 150 nm) morphologies were synthesized from precursor suspensions containing the same amount of GO as a modifier but different amounts of water. Second, the SOD nanocrystals with different morphologies and sizes were deposited between two GO layers to form the sandwich-type membrane. The performance of the sandwich-type membranes in H 2 /CO 2 gas separation was optimized by tuning the properties of the SOD inner layer. The membrane containing spheroidal SOD nanocrystals showed higher H 2 permeance of 4003 ± 1965 GPU and H 2 /CO 2 selectivity of 45.5 ± 1.7 at 25 °C in comparison to the pristine GO membrane (1642 ± 145 GPU and H 2 /CO 2 selectivity of 11.2 ± 2.1).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Naseeb Ullah,Zhaoqi Song,Wei Liu,Chi-Ching Kuo,Aymeric Ramiere,Xingke Cai
Controlled synthesis of noble metal nanoparticles with well-defined size and good dispersion on supports has been a long-standing challenge in heterogeneous catalysis. Here we report a facile photo-assisted H 2 in situ reduction process to synthesize monodispersed Pd nanoparticles with 2–4 nm size on photo-insensitive Sm 2 O 3 rare-earth metal oxide with nanorod morphology. Thanks to the contribution of UV irradiation, the photoelectrons generation in the Sm 2 O 3 support accelerates the H 2 reduction of Pd 2+ ions into Pd 0 and stabilize the growth of very small Pd nanoparticles homogeneously dispersed on the support. The homogeneous distribution of the Pd NPs on the surface of Sm 2 O 3 is most likely attributed to the profuse nucleation sites created by the UV irradiation and the abundance of hydroxyl groups on the support. The hydrogenation of styrene to ethylbenzene was studied as a model reaction. As a result, the UV radiated sample shows an excellent TOF value of 7419 h −1 , which is quadruple of the sample without UV irradiation, under the condition of 0.1 MPa H 2 at a content of 1.0 wt% Pd. Besides, UV radiated sample shows a negligible performance degradation during the repeated cycling process. This photo-promoted H 2 reduction process provides a convenient and straightforward route for assembling materials with novel structures and functions for nanotechnology applications.
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APPLIED SURFACE SCIENCE
·
2019
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IF 5.155
Jin Zhang,Yuyang Huang,Tao Nie,Rui Wang,Beibei He,Bo Han,Huanwen Wang,Yongshang Tian,Yansheng Gong
Herein, self-assembly of hierarchical multihole g-C 3 N 4 hexagon with excellent specific surface area (129 m 2 /g) and nitrogen vacancies were accomplished via a one-step polymerization of hydrothermal-treated dicyandiamide and ethylene-diamine-tetra-acetic acid (EDTA). The special chelate structure of EDTA efficiently enlarged a broad visible light response range, and the concentrations of EDTA promoted the self-assembly formation of different surface morphology . The photocatalytic H 2 production rate under visible light for the optimal g-C 3 N 4 hexagon (CN-20E) reaches 5839 μmol·g − 1 ·h − 1 and its apparent quantum efficiency reaches up to 7.3% at 420 nm, which has a 102 times higher for H 2 production rate than that of bulk g-C 3 N 4 (57 μmol·g − 1 ·h − 1 ). Special structure of the multihole hexagon endows them with remarkably visible light absorption, fast separation of photo-induced charge carriers, large surface areas as well as the exposure of potential photocatalytic active sites, thereby dramatically improved the H 2 production property. Moreover, the forming process for the specific structure and the reaction mechanism of the enhanced photocatalytic activity were proposed according to the experimental results and theoretical calculations. This work exhibits a new avenue to rehandle graphitic carbon nitride precursor to build a grafted structure for developing highly efficient g-C 3 N 4 in the practical photocatalytic application.
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JOURNAL OF SOLID STATE CHEMISTRY
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2019
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IF 2.291
Ruoqian Zhang,Yuanyuan Liu,Jiajia Wang,Zeyan Wang,Peng Wang,Zhaoke Zheng,Xiaoyan Qin,Xiaoyang Zhang,Ying Dai,Baibiao Huang
A triazine-based MOFs [PCN-9(Co)] was synthesized and its photoelectrical, photophysical properties were studied. As a new photocatalyst , PCN-9(Co) displays photocatalytic hydrogen evolution from water under UV–Visible light irradiation . With the introduction of platinum complex, PCN-9-Pt was obtained and platinum complex was believed to coordinate with the N in triazine . The H 2 evolution rate of PCN-9-Pt is greatly improved, about 6.8 times higher than that of PCN-9(Co). The reason is due to the fact that platinum complex plays an important role in improving the separation efficiency of photogenerated charge carriers, as verified by PL and EIS results. This result provides a new kind of idea of modifying MOFs materials with molecular complex to improve the photocatalytic activity .
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