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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

High-efficiency recovery of palladium and platinum using black phosphorus for in-situ synthesis of long-term stable hydrogen evolution catalysts

Rui Gao,Xin Wang,Xue Zhang,Shumeng Zhang,Xinxin Li,Xue-Feng Yu,Licheng Bai

The reserves of palladium (Pd) and platinum (Pt) are scarce and require sophisticated processing. Herein, a three-stage recovery process with black phosphorus (BP) is established in this study to recover Pd and Pt from spent catalysts, presenting a promising strategy for addressing the precious metals crisis. The recovery efficiency of Pd is 99.36 % ± 0.08 % after two stages, with a total recovery capacity of 1426.11 ± 1.73 mg Pd g −1 BP, which is 90 times higher than that of the latest technologies. The overall recovery efficiency of Pt (II) is 98.62 % (467.91 mg Pt g −1 BP) after the third stage (45 °C, 30 min). Furthermore, the current density of the optimal catalysts generated in the first stage (weight ratio: Pd:Pt = 4.9:1) is the highest (57.61 mA cm −1 ; overpotential = 70 mV vs. RHE) among the catalysts generated in the second (Pd:Pt = 1:1) and third (Pd:Pt = 1:11) stages. Pd/Pt–BP generated in the first stage further achieved remarkable long-term stability of 225 h (10 mA cm −2 ) and exhibited maximum durability of > 400 h. Owing to the reduced capability and activation of BP to metals, immobilized Pd (II) and Pt (II) are recovered and directly converted to long-term stable hydrogen evolution catalysts without complex processing.

研究领域: 材料科学 · 催化化学 · 环境工程
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Nano Research · 2023 ·Vol. 16 ·期 5 ·6568-6576 · IF 9.9

Face-to-face heterojunctions within 2D/2D porous NiCo oxyphosphide/g-C3N4 towards efficient and stable photocatalytic H2 evolution

Zhang Genrui,Li Xiaojing,Li Na,Wu Tingting,Wang Lei

Constructing 2D/2D face-to-face heterojunctions is believed to be an effective strategy to enhance photocatalytic performance due to the enlarged contact interface and increased surface active sites. Herein, 2D porous NiCo oxyphosphide (NiCoOP) was synthesized for the first time and coupled with graphitic carbon nitride (g-C 3 N 4 ) nanosheets to form 2D/2D heterojunctions via an in-situ phosphating method. The optimal 4 wt.% 2D/2D NiCoOP/g-C 3 N 4 (OPCN) photocatalyst achieves a hydrogen evolution rate of 1.4 mmol·h −1 ·g −1 , which is 33 times higher than that of pure g-C 3 N 4 . The greatly improved photocatalytic performance of the composite photocatalysts could be attributed to the formation of interfacial surface bonding states and sufficient charge transfer channels for accelerating carrier separation and transfer and the porous structure of NiCoOP nanosheets with abundant surface active sites for promoting surface reactions. Amazingly, the 2D/2D OPCN composite photocatalysts also exhibit superior stability during photocatalytic reactions. This study not only designs new noble-metal-free NiCoOP/g-C 3 N 4 composite photocatalysts but also provides a new sight in fabricating face-to-face 2D/2D heterojunctions for their application in energy conversion areas.

研究领域: 材料科学 · 能源转换 · 催化化学
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JOURNAL OF APPLIED PHYSICS · 2022 ·Vol. 132 ·期 18 · IF 2.877

The introduction of carbon nanosheet buffer layer for enhanced hydrogen evolution performance of C3N4/CoP photocatalysts

Zheng Xiaochun,Ren Shoutian,Gai Qixiao,Wang Yidi,Liu Wenjun

Various defects of nanocomposites inevitably bring some harmful effects on their photoelectric performance, especially considering that interface defects seriously hinder the carrier interfacial transfer. Here, the interface optimization can be realized between graphitic carbon nitride (C 3 N 4 ) and CoP co-catalyst by the introduction of good conductive carbon nanosheets (CNs). As a result, the defect density of synthesized C 3 N 4 /CNs/CoP is reduced to 1.40 × 10 12  cm −3 from 2.55 × 10 12  cm −3 of C 3 N 4 /CoP, and its interface impedance is correspondingly reduced to 34% of that of C 3 N 4 /CoP. Therefore, the optimal H 2 evolution rate of 5.26 mmol g −1  h −1 and apparent quantum efficiency of 9.27% at 420 nm are realized, which are 4.8 and 8.1 times that of C 3 N 4 /CoP photocatalyst in the absence of CNs, respectively. This work provides a general solution to reduce defect density and carrier transfer resistance in nanocomposites by the introduction of a highly conductive buffer layer.

研究领域: 材料科学 · 光催化 · 能源科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Engineering highly active Ag/Nb2O5@Nb2CTx (MXene) photocatalysts via steering charge kinetics strategy

Chao Peng,Xi Xie,Wenkang Xu,Tao Zhou,Ping Wei,Jianbo Jia,Kun Zhang,Yonghai Cao,Hongjuan Wang,Feng Peng,Rui Yang,Xiqiang Yan,Hui Pan,Hao Yu

Steering charge kinetics is one of the most urgent unsolved issues in photocatalysis. The effective spatial separation of photogenerated electron-hole pairs is particularly important in the design and controllable preparation of nano-photocatalysts. Herein, one-dimensional Nb 2 O 5 nanorod arrays with [0   0   1] orientation were grown in-situ on two-dimensional Nb 2 CT x MXenes through a facile hydrothermal method for the first time. Ag nanoparticles were then photodeposited on the Nb 2 O 5 nanorods to form hierarchical 0D/1D/2D nanohybrids. It was experimentally demonstrated that OH is predominantly adsorbed on Nb 2 CT x as termination groups, which resulted in a low work function (2.7 eV). Thanks to the unique structure, the highly active [0   0   1] Nb 2 O 5 nanorods afford high-efficiency photogeneration of electron-hole pairs, while the low-work-function OH terminated Nb 2 CT x allows for trapping holes, and Ag nanoparticles act as electron reservoir and sites of hydrogen evolution reaction (HER). The ternary Ag/Nb 2 O 5 @Nb 2 CT x nanohybrids reached a record HER activity (682.2 and 824.2 μmol·g -1 h −1 use methanol and glycerol as sacrificial agents, respectively) among the niobium-based photocatalysts, demonstrating the potential of MXenes as a platform for the synthesis of high-performance heterojunction structures, where the tunable electronic property is a key factor.

CAS / MDL: 12069-94-2
研究领域: 材料科学 · 化学工程
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CERAMICS INTERNATIONAL · 2020 · IF 3.83

Oxygen-defects modified amorphous Ta2O5 nanoparticles for solar driven hydrogen evolution

Yong Liu,Weixuan Zeng,Yongjin Ma,Rui Dong,Pengfei Tan,Jun Pan

An oxygen-deficient amorphous Ta 2 O 5 nanoparticle photocatalyst was synthesized by a solvothermal method and thermal annealing in Ar atmosphere. The as-prepared Ta 2 O 5 photocatalysts possess improved hydrogen evolution activities compared to pristine Ta 2 O 5 and commercial Ta 2 O 5 under the irradiation of simulated solar light. Therein, Ta 2 O 5 nanoparticles annealing at 400 °C exhibit the most preferable catalytic performance of 10.67 μmol g −1  h −1 . The enhanced performance can be attributed to the existence of oxygen defects in the samples, which can facilitate the separation and migration of photogenerated carriers thereby reducing the probability of recombination.

研究领域: 材料科学 · 可再生能源
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

High-efficient precious-metal-free g-C3N4-Fe3O4/β-FeOOH photocatalyst based on double-heterojunction for visible-light-driven hydrogen evolution

Shu-ao He,Wei Li,Xiao Wang,Qiong Ma,Min Li,Wei Xu,Xue-chuan Wang,Chen-hui Zhao

The two-dimensional (2D) g-C 3 N 4 has a wide application prospect in photocatalysis field due to its larger surface reactions, wider absorption of light and faster charge separation. However, the lack of active site of reduction leads to its poor hydrogen evolution reaction (HER) activity. In this work, the intermediate β-FeOOH was synthesized as a high-efficiency precious metal free co-catalyst in hydrogen production. Then, the g-C 3 N 4 -Fe 3 O 4 /β-FeOOH (CNFF-x,y, x = 1, 2 and 3, y denotes the reaction time (h)) photocatalyst based on p-n and Z-scheme heterojunction was constructed via a subsequent solvothermal process. The chemical composition, microtopography, crystallography, photochemical and electrochemical properties of the CNFF-x,y were analyzed by XRD, FI-IR, TEM, XPS and so on. The visible-light-driven (VLD) catalytic performance of CNFF-x,y heterojunction was evaluated by the hydrogen evolution reaction (HER). Results showed that CNFF-2,10 photocatalyst based on p-n (g-C 3 N 4 -Fe 3 O 4 ) and Z-scheme (Fe 3 O 4 /β-FeOOH) heterojunction presented the highest VLD catalytic HER activity (33.25 μmol g −1  h −1 ) at the absence of Pt co-catalyst after illumination for 6 h. It indicated that the effective introduction of Fe 3 O 4 /β-FeOOH nanoparticles (NPs) into g-C 3 N 4 to construct double-heterojunction (g-C 3 N 4 -Fe 3 O 4 /β-FeOOH) could greatly broaden the light response property and inhibit the recombination of photo-induced carriers, exhibiting enhanced HER activity. Meanwhile, this double-heterojunction photocatalyst presented robust photostability and reproducibility even been used several times. The findings of an intermediate β-FeOOH were put forward in this study will provide some new ideas for the research of HER.

研究领域: 材料科学 · 光催化 · 能源化学
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CHEMICAL PHYSICS LETTERS · 2022 · IF 2.719

Electrospun nano-Ru doped carbon nanofibers for efficient alkaline hydrogen evolution reaction

Ruilin He,Pan Yang,Qingsong Huang,Lijun Yang

While noble metals exhibit excellent electrocatalytic properties, rare elements in the earth's crust. Therefore, reducing the content of noble metals in electrocatalysts is crucial in large-scale electrochemical hydrogen evolution. In this paper, Ru-doped mesoporous carbon nanofibers (Ru- m CNFs) electrocatalysts are prepared by simple electrospinning technology and carbonization strategy. The effects of metal contents on electrocatalytic performance are discussed. With the Ru content of 1.26 %, Ru- m CNFs exhibit the overpotential of 39 mV at current density of 10 mA cm −2 under alkaline conditions, which is comparable to the performance of 20 % commercial Pt/C under the same conditions. This work provided a promising noble catalyst with low loading amount in water-splitting devices for large-scale production of hydrogen.

研究领域: 材料科学 · 能源科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Vacancy-induced tensile strain of CdS/Bi2S3 as a highly performance and robust photocatalyst for hydrogen evolution

Meng Li,Huaisuo Yao,Shunyu Yao,Gang Chen,Jingxue Sun

Lattice strain is a new strategy for promoting photocatalytic activity in order to source more sustainable energy. Vacancy-induced strain is an effective tactic for lattice deformation. Herein, a CdS/Bi 2 S 3 heterojunction structure containing sulfur vacancies (CdS/Bi 2 S 3 -V S ) is synthesized by a one-step solvothermal method. When there are sulfur vacancies in the Bi 2 S 3 lattice (Bi 2 S 3 -V S ), the surrounding atoms move toward sulfur vacancies. This phenomenon lengthens the bonds between surrounding atoms, resulting in tensile stress. Strain engineering adjusts the energy band structure to reduce the interface barrier height, thus effectively improving the interface charge transfer rate. Moreover, density functional theory (DFT) calculations explore the influence of different strain levels on the band structure and Gibbs free energy. The strain-regulated band structure provides a new approach and effectively reduce the interface barrier.

研究领域: 材料科学 · 能源科学
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Journal of Materials Chemistry A · 2016 ·Vol. 5 ·期 6 ·2629-2639 · IF 8.262

Three-dimensional tetsubo-like Co(OH)2 nanorods on a macroporous electrically conductive network as an efficient electroactive framework for the hydrogen evolution reaction

Xin Tong,Dajun Wu,Chi Zhang,Kenan Lian,Dayuan Xiong,Shaohui Xu,Yiping Zhu,Ruijuan Qi,Rong Huang,Lianwei Wang,Paul K. Chu

Conducting the hydrogen evolution reaction (HER) in an alkaline environment using a non-precious transition metal catalyst with high efficiency is challenging. Here, we report excellent HER activity achieved using three-dimensional (3D) tetsubo-like Co(OH)2 nanorods on a macroporous electrically conductive network (MECN) synthesized by a hydrothermal method. This unique framework comprises three levels of porous structures, including a bottom-ordered MECN substrate, an intermediate layer of vertically porous Co(OH)2 nanowires with a mean diameter of 100 nm and length of about 2 μm, and outmost Co(OH)2 nanosheets (≈20 nm). The 3D array structure with a large aspect ratio provides a large specific surface area and exposes more active sites to catalyze electrochemical reactions at the electrode–electrolyte interface. Compared with Co(OH)2 nanosheets on an MECN and foamy Co(OH)2 on an MECN structure, the synthesized architecture has excellent HER catalytic reactivity, including a low potential of −69.2 mV vs. RHE, a cathodic current density of 10 mA cm−2, a small Tafel slope of 61.9 mV dec−1, a high current density, and robust catalytic stability in 1 M KOH, and is promising in HER applications.

CAS / MDL: 12125-02-9 7718-54-9
研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Enhanced photocatalytic hydrogen production through p-n heterojunction interface engineering using Prussian blue analogue-derived Co–Cu–P with graphdiyne (g-CnH2n-2) crystalline/amorphous

Xu Kong,Kai Wang,Zhiliang Jin

More efficient hydrogen production can be achieved by rationally designing heterojunction photocatalysts and constructing interactions between photocatalysts. Herein, The CoP/Cu 3 P (Co–Cu–P) nanocubes were designed using Prussian blue analogue (PBA) as a template through the calcination phosphating method. The novel crystalline-amorphous Co–Cu–P/GDY p-n heterostructures photocatalyst was prepared by a stir-assisted low-temperature water bath method. Under visible light irradiation, the hydrogen evolution efficiency of the Co–Cu–P/GDY-3 heterostructures reached 4790.0 μmol g −1  h −1 , surpassing that of GDY (523.9 μmol g −1  h −1 ) and Co–Cu–P (2458.5 μmol g −1  h −1 ). The remarkable hydrogen evolution activity of the composite catalyst can be attributed to the presence of p-n heterojunction, while the crystalline-amorphous structure promotes efficient interfacial charge transfer. Additionally, the rough and porous nature of the Co–Cu–P/GDY heterostructures surface facilitates mass transfer and hydrogen diffusion during photocatalysis. The charge transfer pathway of the p-n heterojunction was confirmed through various characterizations, including photoluminescence spectroscopy (PL), ultraviolet photoelectron spectroscopy (UPS), valence band X-ray photoelectron spectroscopy (VB-XPS), density functional theory (DFT) calculations, and other relevant techniques. This study offers a fresh perspective on designing PBA derivatives with graphdiyne (GDY) to construct heterostructure photocatalysts for enhanced photocatalytic performance.

CAS / MDL: 10125-13-0
研究领域: 材料科学 · 光催化 · 能源化学
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 22 ·10490-10496 · IF 9.931

Co-doped Ni3S2@CNT arrays anchored on graphite foam with a hierarchical conductive network for high-performance supercapacitors and hydrogen evolution electrodes

Feifei Wang,Yanfang Zhu,Wen Tian,Xingbin Lv,Hualian Zhang,Zhufeng Hu,Yuxin Zhang,Junyi Ji,Wei Jiang

Engineering the surface structure and constructing a suitable internal conductive network is essential for the electron transfer rate and the active material utilization efficiency of an electrode. Here, high-porosity carbon nanotube (CNT) arrays grown on graphite foam (GNF) are synthesized via the self-sacrificial ZnO nanorod template. Then three-dimensional Co-doped Ni3S2 nanostructures (Co–Ni3S2) are coated on the CNT surface via a simple hydrothermal process. The CNTs/GNF hybrid with a hierarchical conductive network exhibits good electrical conductivity, while the tectorum-like Co–Ni3S2 nanosheet structure may facilitate both the ion and electron transfer in the redox process. Therefore, the Co–Ni3S2@CNTs/GNF composite shows a highest specific capacitance of 4.1 F cm−2, good rate performance (57.8% capacitance retention from 1 to 40 mA cm−2) and cycling stability (89.8% capacitance retention after 1000 cycles). Moreover, the Co–Ni3S2@CNT/GNF electrode also reveals good hydrogen evolution reaction activity in alkaline solution (an overpotential of 155 mV at 10 mA cm−2).

CAS / MDL: 1314-13-2
研究领域: 材料科学 · 电化学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Dual electron transfer routes in core-shell double Z-scheme artificial photosynthetic system for improved photoredox activity

Jie Hu,Xiuwu Xu,Xin Wei,Maobin Xiao,Weiran Wu,Zhaoyu Wang,Lele Wang,Qinqin Liu

Developing artificial photosynthetic system with high activity is significant for long-term solar light conversion. Inspired by the natural Z-scheme photosystem, a ternary core-shell ZnIn 2 S 4 /MoO 3 /MoS 2 (ZOS) composite with double Z-scheme junction was prepared by in-situ vulcanization of MoO 3 nanosheets . Such in-situ formed intimate interfaces can overcome the high interfacial charge transfer barrier between different composites thus boosting the charge separation efficiency. The dual Z-scheme heterojunction provided dual electron transfer routes and favored the charge transfer. In addition, the ternary core-shell structure offered more spatially separated active sites which also increased the photocatalytic activity. Profiting from these strategies, the optimized ZOS-1 sample afforded 3.71 mmol·g −1 ·h −1 hydrogen evolution rate at 420 nm, which was 18.5 and 2.5 times higher than that of MoO 3 and ZnIn 2 S 4 , respectively. In addition, 88% tetracycline can be eliminated in the solution within 70 min in the presence of ZOS-1 sample. This study provides an effective strategy for designing high-efficiency artificial photosynthetic systems under Z-scheme charge transfer routes in photocatalytic reactions.

研究领域: 材料科学 · 光合作用工程 · 环境科学
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