JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
RuoKun Jia,PengPeng Wang,XiaoHang Yang,DuMin Li,JianGuo Qiao,TianXiang Li,JiaHui Chen
The rational modulation of the Si/Al ratio within molecular sieves holds utmost significance for augmenting photocatalytic activity. In this context, g-C 3 N 4 /HBeta composite photocatalysts were synthesised via a straightforward in situ thermal polymerisation procedure employing HBeta molecular sieves possessing multiple active sites and diverse Si/Al ratios. Through the variation of Si/Al ratios, the adsorption capacity, photogenerated carrier complexation efficiency, and active site characteristics could be effectively manipulated. The catalyst with the smallest Si/Al ratio (HBeta 25 ) exhibited the highest catalytic activity, with a hydrogen production efficiency of 2.346 mmol g⁻¹. This value was 4.9 times higher than that of pure g-C 3 N 4 , and the degradation efficiency of RhB was 3 times that of pure g-C 3 N 4 . The catalytic proficiency was principally validated by employing a comprehensive suite of techniques, including XPS, BET, SEM, and NH 3 -TPD. Our results demonstrate for the first time the strong potential of zeolite Si/Al ratio to modulate the catalytic activity of photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xuechen Zhou,Limo He,Chiyu Wang,Yufan Yang,Yanglin Chen,Song Hu,Sam Fong Yau Li,Yifei Sun,Sheng Su,Yi Wang,Jun Xiang
Methanol, as a H 2 storage carrier, is a good option to tackle with the challenges of H 2 storage and transportation. To improve hydrogen production and reduce energy consumption, a new approach of electrified methanol decomposition (MD) by Joule heating was investigated in this work. The conductive metal skeleton catalysts were prepared using nickel foam (NF) as a catalyst support and employing a hydrothermal-impregnation method to load the Cu/Zn active components. The catalyst heats up rapidly upon energizing, and the heating rates reaches over 10 °C/s. The Joule heating method significantly promotes the methanol conversions of CuO-ZnO/NF, CuO/NF, and ZnO/NF. Methanol conversion over CuO-ZnO/NF at 300 °C under Joule heating is over 80 % higher than that of conventional external heating, while its energy consumption is only 29 % of that under external heating. As a result, methanol conversion per unit power in Joule heating condition increases by 5.6 times compared with that in external heating. The in/ex-situ characterizations reveal that the Joule heating of metal skeleton catalyst promotes the lattice oxygen release of NF skeleton and redox of Cu/Zn species, which generates an extra electrochemical effect on the reaction. This study of Joule heating provides a new strategy of converting methanol to H 2 in a more efficient, energy-saving, and flexible way, and has important application potential in hydrogen energy and chemical energy storage (“Power-to-X”).
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Frontiers of Chemical Science and Engineering
·
2021
·Vol. 16
·期 4
·498-510
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IF 4.204
Bo Jinxiao,Li Mei,Zhu Xinli,Ge Qingfeng,Han Jinyu,Wang Hua
The electrochemical conversion of CO 2 -H 2 O into CO-H 2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H 2 ratio are highly desired. Herein, a series of N -doped carbon nanotubes encapsulating binary alloy nanoparticles (M x Ni-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of mela-mine and metal precursors. The M x Ni-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H 2 ratios, from 0.5:1 to 3.4:1, can be produced on M x Ni-NCNT. More importantly, stable CO/H 2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co 1 Ni-NCNT and Co 2 Ni-NCNT, respectively, over a potential window of −0.8 to −1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H 2 ratio from electrochemical CO 2 reduction.
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ACS Applied Materials & Interfaces
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2014
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IF 5.9
Jie Zhang,Ping Wang,Jian Sun,Yongdong Jin
Solar-driven photocatalytic process based on electron–hole pair production in semiconductors is a long sought-after solution to a green and renewable energy and has attracted a renaissance of interest recently. The relatively low photocatalytic efficiency, however, is a main obstacle to their practical applications. A promising attempt to solve this problem is by combined use of metal nanoparticles, by taking advantage of strong and localized plasmonic near-field to enhance solar absorption and to increase the electron–hole pair generation rate at the surface of semiconductor. Here, we report a semiconductor/metal visible-light photocatalyst based on CdSe/CdS-Au (QD-Au) core–satellite heteronanocrystals, and assemble them on graphene nanosheets for better photocatalytic reaction. The as-synthesized photocatalyst exhibits excellent plasmon-enhanced photocatalytic activities toward both photodegradation of organic dye and visible-light H2 generation from water. The H2 evolution rate achieves a maximum of 3113 μmol h–1 g–1 for the heteronanocrystal-graphene composites, which is about 155% enhancement compared to nonplasmonic QD-G sample and 340% enhancement compared to control QD-Au-G sample, and the apparent quantum efficiency (QE) reaches to 25.4% at wavelength of 450 nm.
研究领域:
材料科学
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纳米技术
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光催化
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可再生能源
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半导体物理
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Journal of Cleaner Production
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2023
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IF 11.1
Shen Xu,Jianying Huang,Zengxing Li,Yonggang Lei,Yingzhen Zhang,Kim Hoong Ng,Yuekun Lai
It is very attractive to find a cheap and efficient cocatalyst for enhancing the H 2 generation of graphitic carbon nitride (CN) under visible light. To achieve that, we proposed a novel two-step method to deposit sub-10 nm metallic Ni 2 P particles on the surface of CN sheets for a maximized interfacial contact. Characteristic results confirmed the establishment of ohmic heterojunction upon Ni 2 P-modification of CN, which deemed to be an effective measure to alleviate photo-charges recombination. In addition to facilitating spatial separation of charges, Ni 2 P could also enhance the optical properties of CN while reducing its impedance for interfacial electron shuttling. Better still, the P-end of Ni 2 P is highly electronegative, offering desirable H + -capturing capability for enhanced H 2 generation. These give rise to an improved H 2 production of Ni 2 P/CN composite, optimally at 645.3 μmol g −1 ·h −1 as compared to immeasurable H 2 yielded by the pristine CN. Such photocatalytic performance is even comparable to the Pt-modified CN photocatalyst (640.6 μmol g −1 ·h −1 ). In recyclability test, a notable activity suppression of 33.17% was recorded after four reaction cycles. This can be ascribed to the pronounced photo-corrosion of the Ni 2 P cocatalyst during photoreaction. Nonetheless, a remarkably high H 2 generation (1328.6 μmol g −1 in 3 h) was still attained at 4 th cycle. This justifies the effectiveness of our synthesized Ni 2 P cocatalyst in enhancing H 2 generation of CN under visible light irradiation.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Feng Shi,Hongyuan Wang,Yifei Chen,Yanling Lu,Defa Hou,Can Liu,Yi Lu,Xu Lin,Xiaoqin Yang,Zhifeng Zheng,Yunwu Zheng
To develop an efficient and feasible catalyst for converting inedible vegetable oil to green biodiesel via a one-step decarboxylation process, a series of Ni-based MgO-Al 2 O 3 catalysts with different active Ni species were fabricated by adjusting the various Ni loading amounts (2.5–20%) and applied to the catalytic deoxygenation of OA to generate green biodiesel. Additionally, the structure-property relationship, deactivation mechanism and regeneration performance were also evaluated via various characterization technologies (XRD, BET, NH 3 -TPD, H 2 -TPR, XPS, SEM-EDX, HRTEM, TGA, Raman as well as GC/MS and UV-fluorescence spectra). The experimental results indicated that Ni introduction obviously enhanced the conversion ratio. Ni (10%)/MgO-Al 2 O 3 catalysts exhibited excellent catalytic performance with the highest HCs (95.12%), olefin content (57.37%) and green biodiesel content (75.90%) due to mild Brønsted-rich acidity sites, lower reduction temperature, higher active metallic Ni species content, suitable oxygen vacancy content and favorable texture properties via the decarbonylation reaction pathway. Furthermore, lower Ni loading was beneficial to gasoline and bioaviation fuel generation due to higher Brønsted-rich acidity sites and total acid amount, which boosted C-C scission by cracking reaction, and higher Ni content facilitated biodiesel formation. Additionally, Ni (10%)/MgO-Al 2 O 3 catalysts showed excellent reusability and regeneration due to Ni active species, but these advantages were slightly decreased (HCs: from 95.12% to 61.63%; biodiesel: from 75.90% to 57.52%) due to coke deposition and metal active species leaching and oxidation .
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Nano Energy
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2022
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IF 19.069
Manyi Gao,Fenyang Tian,Xin Zhang,Yequn Liu,Zhaoyu Chen,Yongsheng Yu,Weiwei Yang,Yanglong Hou
Reinforcing the charge separation and transfer in layered polymeric carbon nitride (PCN) is the key issue to enhance its photocatalytic activity but still remains very challenging. Herein, for the first time, the synergetic Pd single atoms (PdSAs) and carbon-supported Pd nanoparticles (NPs) are introduced into the interlayer and surface of layered PCN respectively to address this challenge. The PdSAs are in intimate contact with the adjacent PCN layers and serve as interlayer charge transfer channels, while the carbon-supported Pd NPs contribute to multistep PCN-carbon-Pd NPs Schottky junctions on PCN surface. Experiments and theoretical calculations demonstrate that such unique architectures provide intrinsic driving force to extract the electrons from PCN to outermost Pd NPs with high migration rate via vertical PdSAs channels. This directional charge transfer in PCN greatly expedite the separation of charge carriers in both inner and surface of PCN and simultaneously yield electron-rich Pd NPs active sites with optimized H 2 adsorption energy , thus leading to improved intrinsic H 2 evolution reaction kinetics. Consequently, the Pd/PCN 2 performs ultrahigh photocatalytic H 2 evolution rate of 83.34 mmol g −1 h −1 in the dispersed particulate system and 100.4 mmol h −1 m −2 in the film form under simulated sunlight. This work provides a new promising approach to engineer the spatial charge transfer behaviors for high-performance PCN-based photocatalysts .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Xiaohui Ma,Wenjun Li,Hongda Li,Mei Dong,Xinyang Li,Liang Geng,Hongxia Fan,Yanyan Li,Hong Qiu,Tianyu Wang
Here, we synthesized a series of noble-metal-free MoP/In 2 S 3 Schottky heterojunction photocatalysts through two-step synthesis. Morphology characterization revealed that In 2 S 3 was deposited on metal-like MoP. The electrochemical experiment, photoluminescence (PL) and time-resolved transient PL results verify that electron-hole pairs separation efficiency of MoP-In 2 S 3 composites has been immensely elevated compared to pristine In 2 S 3 . The effective separation of photocarriers is attributed to the appropriate Schottky energy barrier, band bending and Fermi level rearrangement between MoP and In 2 S 3 . Furthermore, the X-ray photoelectron spectra confirmed that electrons transferred from In 2 S 3 to MoP in Schottky heterojunction. Importantly, MoP possesses active sites for H 2 generation resulting from nearly zero binding for H atoms and low onset overpotentials. As expected, the 25 %MoP-In 2 S 3 composites exhibited excellent photocatalytic activity (481.73 μmol·h −1 ·g −1 ), which was about 23 times than In 2 S 3 -1 %Pt (20.73 μmol·h −1 ·g −1 ). Hence, the enhanced photocatalytic performance was ascribed to not only the formed Schottky heterojunction leading to better charge separation, but also MoP as the active sites accelerated the surface proton reduction reaction. The research furnishes a thought that suitable semiconductors and metal-like were selected to construct high performance and low-cost Schottky heterojunction with efficient charge separation and active sites for resultful photocatalytic H 2 generation.
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高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
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IF 5.141
Hao Zhang,Hongjie Zhu,Haitao Zhao,Mingyu Dou,Xingliang Yin,Hua Yang,Dacheng Li,Jianmin Dou
Photocatalytic water splitting to produce hydrogen has gradually become a research hotspot in recent years, and molecular cocatalysts especially cobalt-based complexes as proton reduction cocatalysts have attracted wide attention due to their high activity and selectivity. In this study, CdS nanorods were employed as photosensitizers, and a novel dinuclear cobalt-bis(thiosemicarbazone) complex with definite structure was used as a cocatalyst to improve visible-light-driven hydrogen evolution. Under the optimum conditions, this noble metal-free system exhibited an average hydrogen evolution rate of 1045 μmol·h −1 in 8 h irradiation. This system could work for 24 h with a TON of 16,400, and the average apparent quantum yield of this system is ∼21% at 420 nm. On the basis of photoelectrochemical studies and electrochemical analysis, we proposed a possible mechanism for hydrogen production in this three-component system.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Youzhou He,Mingzuo Chen,Yao Jiang,Lei Tang,Jianning Yu,Ya Chen,Min Fu,Xuemei Tan,Jiajia Jing,Guizhi Zhang,Xingyan Liu
The modification of graphite carbonitride (g-C 3 N 4 ) is beneficial to increase its specific surface area and high quantum efficiency, thus improving its activity. Herein, the Yb 2 O 3 /g-C 3 N 4 composites were adjusted through dual regulation synergistically (nanostructure design of g-C 3 N 4 and addition of lanthanide oxides Yb 2 O 3 ) to improve the photocatalytic performance of hydrogen production and NO removal simultaneously. The as-prepared 1% Yb 2 O 3 /tubular g-C 3 N 4 could efficiently promote the photocatalytic hydrogen evolution (4071.763 μmol·g −1 ·h −1 ) and NO removal performance (54.20%), which was approximately 8.85 times and 32.01% higher respectively than that of bulk g-C 3 N 4 prepared by melamine (g-C 3 N 4 -M). The formation process of·O 2 - and·OH radicals and the oxidation process of NO had been systematically studied through ESR and in-situ DRIFTS , which proved that the coupling of tubular g-C 3 N 4 with Yb 2 O 3 had a positive effect. This work provided a novel strategy for dual regulation (adjust morphology and metal oxide introduction) synergistically design of bifunctional photocatalysts to enhance H 2 production and NO removal simultaneously.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Pengpeng Zhang,Chao Xue,Yukun Li,Shuaiwei Guo,Xilai Zhang,Peng Zhang,Guosheng Shao
High-efficiency light utilization and prolonged lifetime of photo-induced charge carriers is a key step towards superior photocatalytic H 2 evolution. Herein, the design of a novel spatially separated Ni 2 P co-catalyst decorated SiO 2 /rGO/Cd 0.5 Zn 0.5 S yolk-shell structural photocatalytic nanoreactor is reported. In this system, the advantages of ultrathin mesoporous shell and yolk-shell structure not only facilitate the mass diffusion with short length, but also allow broad-spectrum light absorption and increase the density of catalytic active sites. Importantly, the photo-generated electrons can be directionally injected from the outermost Cd 0.5 Zn 0.5 S shell to the spatially separated Ni 2 P co-catalyst. The dynamic behaviors of photo-induced charge carriers can be rationally regulated by the suitable energy level alignment and the built-in electric fields derived from both sides of embedded rGO interlayer. The synergistic effects of the excellent light-harvesting ability, more exposed active sites and improved charge separation efficiency significantly boosted the photocatalytic performances of hydrogen evolution. As a result, the optimal SiO 2 /Ni 2 P/rGO/Cd 0.5 Zn 0.5 S composite exhibited the highest hydrogen generation of 11.65 mmoL‧g −1 ‧h −1 , even after five cycles. This work proposes new insights into the design of the efficient hollow sphere structural heterojunctions for photocatalytic water splitting applications.
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Green Energy & Environment
·
2020
·
IF 6.395
Zhaoning Song,Juncong Yuan,Zhenping Cai,Dong Lin,Xiang Feng,Nan Sheng,Yibin Liu,Xiaobo Chen,Xin Jin,De Chen,Chaohe Yang
The advocacy of green chemical industry has led to the development of highly efficient catalysts for direct gas-phase propene epoxidation with green, sustainable and simple essence. The S-1/TS-1@dendritic-SiO 2 material with three-layer core–shell structure was developed and used as the support for Au catalysts, which showed simultaneously fantastic PO formation rate, PO selectivity and stability (over 100 h) for propene epoxidation with H 2 and O 2 . It is found that silicalite-1 (S-1) core and the middle thin layer of TS-1 offer great mass transfer ability, which could be responsible for the excellent stability. The designed dendritic SiO 2 shell covers part of the acid sites on the external surface of TS-1, inhibiting the side reactions and improving the PO selectivity. Furthermore, three kinds of SiO 2 shell morphologies (i.e., dendritic, net, mesoporous shell) were designed, and relationship between shell morphology and catalytic performance was elucidated. The results in this paper harbour tremendous guiding significance for the design of highly efficient epoxidation catalysts.
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