CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yunxiao Zhang,Qingxiang Cao,Xuelian Wu,Yonghao Xiao,Aiyun Meng,Qitao Zhang,Yuxiang Yu,Wei-De Zhang
Establishing effective non-platinum active sites on polymeric carbon nitride (PCN) remains a great demanding to achieve highly efficient photocatalytic hydrogen generation performance. Modification with molecular complex catalysts on PCN skeletons has been demonstrated as a promising strategy. Herein, hybrid photocatalytic material was successfully synthesized by modifying PCN with copper molecular ligand ( CuL, Schiff-based copper complex) via π-π stacking. Interestingly, atomically dispersed Cu is formed in CuL/PCN. Compared to PCN, the π-π stacking in CuL/PCN is beneficial for facilitating the migration of photogenerated electrons from PCN to CuL . Furthermore, photo-redox ability of the atomically dispersed Cu is regulated by the ligand (Schiff base) in CuL and the introduction of CuL provides abundant active sites to capture the photogenerated electrons, whereby the reductive reaction of H 2 O/H + to H 2 for CuL/PCN was significantly promoted. Consequently, an optimal hydrogen evolution rate of 15.90 μmol·h −1 was obtained on 3CuL/PCN, which was 2.02 times higher than that of 3.0 wt% Pt/PCN (7.86 μmol·h −1 ). More importantly, the hybrid material exhibits an outstanding conversion efficiency (90 %) and selectivity (99 %) for α-methylation of ketones by making full use of the in-situ generated H species and photogenerated holes under visible light irradiation.
研究领域:
材料科学
·
催化
·
光化学
·
无机化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Limin Guo,Runze Hu,Caifu Zhong,Xinxin Wang,Jiaming Liu,Xiaohui Wang
An elegant templating method has been developed for the rational design and synthesis of hierarchical SnS 2 nanoclusters composed of ultrathin nanosheets and embedded inside TiO 2 nanoporous arrays. Herein, benefiting from their unique structural merits and metal-like plasmonic activity, the TiO 2 @SnS 2 heterostructures exhibit enhanced photocatalytic H 2 evolution properties in terms of good cycling performance. S vacancies and N-doping are proved to be vitally important to the electronic structures and bandgap of SnS 2 , thus influence the plasmonic property and separation of photo-carriers. The optimized TiO 2 @6nmSnS 2 /N nanoporous arrays give an ultra-high H 2 yield rate of 285 μmol h −1 cm −2 under a low catalyst loading mass, that comparable to most noble metal catalysts . Remarkable cycling performance with a capability retention of 90% is achieved after 30 h under solar light illumination. As an innovative exploration, this study demonstrates that the photocatalytic activities of nonmetal, earth-abundant SnS 2 can be enhanced with plasmonic effect, which may serve as an excellent catalytic agent for solar energy conversion to chemical fuel.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·Vol. 51
·期 25
·46911-46917
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IF 5.6
Pengxin Xu,Zili Zhou,Yaqi Wang,Ergeng Zhang,Zhanyong Wang,Ding Zhou
Highly transparent ceramics of Zr 4+ and Sc 3+ ions co-doped 5 at.%Yb: Lu 2 O 3 were prepared by using wet-chemical precipitant method combined with pressureless sintering in flowing H 2 atmosphere, where Zr 4+ was induced as the sintering aid and Sc 3+ as the band regulators to realizing spectral broadening of Yb:Lu 2 O 3 . The microstructure, broad emission band, PL spectrum and optical properties of the Zr 4+ and Sc 3+ co-doped 5 at.%Yb:Lu 2 O 3 ceramic samples were investigated by SEM, XRD, PL spectrum and other characterization methods. The results indicate that the maxim FWHM of the excitation emission spectrum of Yb:(Lu X Sc 1-X ) 2 O 3 ceramic is 15 nm when x = 0.5. Furthermore, the incorporation of Zr 4+ at a doping concentration of 2 at.% alleviated the microstructural inhomogeneity of the Yb:(Lu 0.5 Sc 0.5 ) 2 O 3 ceramics and significantly reduced the grain size, resulting in high transparency of up to 81.2 % at 1200 nm wavelength. These findings demonstrate a great potential of this ceramic for applications in ultrafast short pulse laser media.
研究领域:
材料科学
·
陶瓷
·
激光材料
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光学性能
·
固态物理
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
·
2021
·Vol. 7
·期 47
·
IF 14.143
Zhong Liang,Lianpeng Song,Mingzi Sun,Bolong Huang,Yaping Du
Electrochemical reduction of CO 2 (CO 2 RR) to value-added liquid fuels is a highly appealing solution for carbon-neutral recycling, especially to syngas (CO/H 2 ). Current strategies suffer from poor faradaic efficiency (FE), selectivity, and controllability to the ratio of products. In this work, we have synthesized a series of single and dual atomic catalysts on the carbon nitride nanosheets. Adjusting the ratio of La and Zn atomic sites produces syngas with a wide range of CO/H 2 ratios. Moreover, the ZnLa-1/CN electrocatalyst generates the syngas with a ratio of CO/H 2 = 0.5 at a wide potential range, and the total FE of CO2RR reaches 80% with good stability. Density functional theory calculations have confirmed that the Zn and La affect electronic structures and determine the formation of CO and H 2 , respectively. This work indicates a promising strategy in the development of atomic catalysts for more controllable CO 2 RR.
研究领域:
电化学
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催化
·
材料科学
·
环境科学
·
能量转换
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Xiangchen Kong,Huiming Huang,Zhaoyang Li,Yanqin Liang,Zhenguo Li,Shengli Zhu
TiO 2 (B) nanosheets/GO (graphene oxide) hybrids are considered to be outstanding performance photocatalysts for high efficiency of H 2 evolution. However, they still suffer severe challenges during the synthetic processes, such as a large amount of the capping agents adhering on the surface and easy occurrence of aggregation. To figure out these obstacles, Ar plasma treatment as a modified method in this study not only enable the TiO 2 (B) nanosheets distributed uniformly on the GO sheets but also engineer defects within TiO 2 (B) nanosheets to significantly improve the photocatalytic activity for the water splitting. The hydrogen evolution rate of the TiO 2- x (B)/GO sheets is 1.4 times higher compared with that of original TiO 2 (B)/GO sheets without Ar plasma treatment. The improved photocatalytic properties were owing to the synergetic effects of oxygen vacancies and the heterojunction between GO and TiO 2 (B), which can promote the visible light utilization and accelerate separation and transportation of photogenerated electron-holes. This study can provide a facile pathway to prepare the two-dimensional hybrid photocatalysts with high photocatalytic H 2 activity.
研究领域:
材料科学
·
纳米科技
·
能源化学
·
光催化
·
二维材料
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Hongqiang Shen,DanDan Shang,Longhua Li,Di Li,Weidong Shi
Full solar-energy utilization and sufficient charge flow supply are highly desired for the rational design over efficient heterojunction photocatalyst. Herein, we introduced 2D Schiff-base covalent-organic frameworks material (COF-TpPa-1) as a photosensitizer and support to integrate with 2D TiO 2 nanosheets of H 2 -evolving semiconductor, establishing a 2D/2D hybrid photosensitive system. The 2D/2D COF-TpPa-1/TiO 2 heterogeneous composite displayed the optimum yield of 1.37 mmol h −1 g −1 under visible light irradiation, which is ∼ 29 times higher than that of pristine COF-TpPa-1. Furthermore, the mass short-distance photoelectron flow through the intimate hetero-interface contact between 2D COF-TpPa-1 and 2D TiO 2 has been evidenced by various characterizations and DFT calculations. This work reported here enables the extension of various 2D/2D hybrid collocations between H 2 -evolving metal oxide semiconductors and photosensitizing COF materials for boosting photocatalytic performance.
研究领域:
材料科学
·
光催化
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Fang He,Hubo Yuan,Huayan You,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
Building carbon nitride (CN)-based core shell heterostructures is an effective strategy to enhance the photocatalytic performance and stability by optimize the interface area and protect the CN core, respectively. Moreover, by fabricating the porous structures in core shells can further optimize the light absorption, charge separation, and mass transfer. Herein, we have constructed porous C-PDA–CN–ms core-shell heterostructures through a facile green molten salt (ms) sculpture the polydopamine (PDA) derived carbon (C-PDA) shells with CN core. In which, the C-PDA-CN core-shells arise from in situ polymerization of dopamine (DA) on the surface of melamine to form PDA@melamine coatings followed by thermal polycondensation . The molten salts at high-temperature act as a green fluid immersing in and out of C-PDA-CN core-shells to further produce porous structures. The 1 wt% C-PDA–CN–ms with porous core-shell structures display photocatalytic H 2 evolution rate of 3830 μmol h −1 g −1 , which is 20.8 times enhancement of 1 wt% C-PDA-CN core-shells, even 73.6 times higher than that of pristine CN. It reveals that the porous and core-shell heterostructures endow C-PDA–CN–ms enhanced light absorption, various charge transport channels for improved charge carrier separation and transfer, contributing to the superior photocatalytic H 2 evolution performance. Our work opens a new window for the green construction of porous core-shell heterostructures of CN-based photocatalysts .
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yixuan Lv,Dandan Ma,Chao Yang,Kunli Song,Le Shi,Yonghong Cheng,Chunming Niu,Jian-Wen Shi
Lead-free halide perovskites have enormous superiority in photoelectric devices, but low photocatalytic hydrogen evolution (PHE) hinders their application in photocatalysis. Here, a heterojunction composed of CsCu 2 I 3 (CCI) perovskite and graphite carbon nitride (CN) is constructed by in-situ hot-injection method for the first time. The resultant CCI/CN presents a significantly enhanced PHE performance from hydroiodic acid (HI) splitting with a PHE rate of 2212 umol/g/h, which is four times higher than CCI and nearly ten times higher than CN. It is revealed that a unique N-I bond is formed by the connection of N in CN and I in CCI at the interface between CN and CCI, which serves as a fast channel for the transfer of photogenerated electrons to establish a type II mechanism, effectively promoting the PHE performance. This study provides ideas and methods for the construction of type II photocatalyst for hydrogen production using lead-free halide perovskite.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Tao Yan,Jianhua Yang,Jinming Lu,Liang Zhou,Yan Zhang,Gaohong He
Recently, pillar-layered MOF materials have attracted much attention and shown great potential in separation application due to their fine pore size/channel and pore surface chemistry tunability and designability. In this work, we reported an effective and universal synthesis strategy for preparing ultra-microporous Ni-based pillar-layered MOF [Ni2(L-asp)2(bpy)] (Ni-LAB) and [Ni2(L-asp)2(pz)] (Ni-LAP) (L-asp = L-aspartic acid, bpy = 4,4′-bipyridine, pz = pyrazine) membranes on a porous α-Al2O3 substrate with high performance and good stability by secondary growth. Through this strategy, the seed size reduction and screening engineering (SRSE) is proposed to obtain uniform sub-micron size MOF seeds by high-energy ball milling-combined solvent deposition. This strategy not only effectively addresses the issue of obtaining the uniform small seeds being significant for secondary growth but also provides an approach for the preparation of Ni-based pillar-layered MOF membranes where the freedom of synthesizing small crystals is lacking. Based on reticular chemistry, the pore size of Ni-LAB was narrowed by making use of shorter pillar ligands of pz instead of the longer pillar ligand of bpy. The prepared ultra-microporous Ni-LAP membranes exhibited a high H2/CO2 separation factor of 40.4 with H2 permeance of 9.69 × 10–8 mol m–2 s–1 Pa–1 under ambient conditions and good mechanical and thermal stability. The superiority of the tunable pore structure and the remarkable stability of these MOF materials showed great potential for industrial H2 purification. More importantly, our synthesis strategy demonstrated the generality for preparation of MOF membranes, enabling the regulation of membrane pore size and surface functional groups by reticular chemistry.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2023
·Vol. 13
·期 13
·8915-8922
·
IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Fang He,Hong Zhong,Meng Wang,Hubo Yuan,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
All carbon-based CG/M − CN rectangular nanotubes have been constructed by a facile molten salt thermal condensation of melamine and glucose. In the molten salt fluid, the glucose is carbonized into graphene-like (CG) nanosheets acting as an electron acceptor , and the melamine thermally condenses into carbon nitride (M − CN) rectangular nanotube acting as an electron donor . The 0.5 wt% CG/M − CN nanotubes display a photocatalytic H 2 evolution rate of 2345 μmol h −1 g −1 , which is 1.52 times higher than that of M-CN. Moreover, without loading Pt co-catalyst, the 0.5 wt% CG/M − CN nanotubes show a 12.75 times higher photocatalytic H 2 evolution rate than that of M-CN. It is revealed that the graphene-like CG nanosheets not only can act as an electron acceptor boosting charge carrier separation, but also function as a HER cocatalyst for M-CN. Our work provides a new insight for the development of all carbon-based photocatalysts for energy-related applications.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Wenxin Liu,Jiabin Zou,Shuni Li,Jinkun Li,Feihu Li,Zili Zhan,Yeguang Zhang
Hydrogen sensors are easily deactivated by hexamethyldisiloxane (HMDSO) poisoning. Moreover, the existing anti-poisoning strategies can also damage the overall sensing performance of these hydrogen sensors. Therefore, a new bilayer design with a Pd/In 2 O 3 sensitive layer and an In 2 O 3 /Al 2 O 3 catalytic filter layer is proposed to avoid the deactivation of hydrogen sensors. The In 2 O 3 /Al 2 O 3 layer helps in hindering HMDSO and its decomposition products from reaching the Pd/In 2 O 3 layer. The H 2 response of the sensors is enhanced due to the small size of In 2 O 3 and the electronic sensitization of Pd. As a result, the bilayer sensors exhibit high response (Ra/Rg = 53) and ultra-fast response time (1 s) towards 3000 ppm H 2 at 365 °C. The resistance and the H 2 response of the bilayer sensors are almost unchanged after 40 min of 10 ppm HDMSO poisoning. In this paper, the mechanism of resistance against silicone poisoning and the H 2 response of the bilayer sensors are discussed from the separation of sensing and catalytic filtration reactions to the behavior of adsorbed oxygen.
✓ 已验证
产品关联
DOI
高影响因子
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