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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Carbonaceous Structures as Electronic Bridges to Enhance Charge Migration and Radical Reactions in Composite Photocatalysts: An Effective Way to Achieve Efficient Mineralization of Pollutants

Ruifeng Zhou,Jiaqi Zhao,Liang Chen,Jingyang Zhang,Zehui Fan,Chong Peng,Yun Li,Shuyi Yang,E Tao

ABSTRACT The intrinsic correlation between photo-induced extraction of hole and free radical reactions can facilitate the mineralization of contaminants via promoting the transfer of electrons from the semiconductor to the solution. TiO 2 /C/g-C 3 N 4 composite photocatalysts are prepared using thermal polycondensation and sol-gel methods in this paper. The introduction of carbon at the interface between the two phases creates charge migration channels that facilitate electron transfer at the interface of semiconductor catalyst as well as collisions of dissolved oxygen to the catalytic sites, which are able to promote catalytic oxidation reactions. Considering Rh-B as target, the removal rate is 97.2±0.2% within 90   min. The involvement of hydroxyl radicals and superoxide radicals is confirmed by carrying out radical quenching experiments and ESR characterization, suggesting that effective electron transfer synergistically promotes the production of hydroxyl radicals. Therefore, it emphasizes the importance of the indeterminate carbon bridged 2D/3D interface for constructing charge migration channels as well as promoting the efficiency of carrier separation in the process of photocatalytic efficient degradation of dyes.

研究领域: 环境科学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

Fabrication of carbon bridged g-C3N4 through supramolecular self-assembly for enhanced photocatalytic hydrogen evolution

Huiliang Li,Fengping Li,Zeyan Wang,Yachen Jiao,Yuanyuan Liu,Peng Wang,Xiaoyang Zhang,Xiaoyan Qin,Ying Dai,Baibiao Huang

Carbon bridged graphitic carbon nitride (g-C 3 N 4 ) was prepared by a facile supramolecular self-assembly method. Experimental results and theoretical calculations indicate C atoms were introduced into the g-C 3 N 4 lattice by substituting the bridged N atoms. As a result, the delocalized big π bonds can be formed among the adjacent heptazine rings, which could both enhance the light absorption and promote the charge separation. Beneficial from the efficient charge separation and enhanced light absorption, the carbon bridged g-C 3 N 4 exhibits high efficient photocatalytic activity, where the H 2 evolution rate is about 7 times as high as that of pristine g-C 3 N 4 . This work demonstrates carbon bridged C 3 N 4 can be fabricated by a simple supramolecular self-assembly process, which could be useful for the further development of high efficient g-C 3 N 4 photocatalysts.

CAS / MDL: 9012-76-4
研究领域: 材料科学 · 光化学 · 纳米技术
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-12 · IF 14.7

Stable hydrogen evolution reaction at high current densities via designing the Ni single atoms and Ru nanoparticles linked by carbon bridges

Yao Rui,Sun Kaian,Zhang Kaiyang,Wu Yun,Du Yujie,Zhao Qiang,Liu Guang,Chen Chen,Sun Yuhan,Li Jinping

Continuous and effective hydrogen evolution under high current densities remains a challenge for water electrolysis owing to the rapid performance degradation under continuous large-current operation. In this study, theoretical calculations, operando Raman spectroscopy, and CO stripping experiments confirm that Ru nanocrystals have a high resistance against deactivation because of the synergistic adsorption of OH intermediates (OH ad ) on the Ru and single atoms. Based on this conceptual model, we design the Ni single atoms modifying ultra-small Ru nanoparticle with defect carbon bridging structure (UP-RuNi SAs /C) via a unique unipolar pulse electrodeposition (UPED) strategy. As a result, the UP-RuNi SAs /C is found capable of running steadily for 100 h at 3 A cm −2 , and shows a low overpotential of 9 mV at a current density of 10 mA cm −2 under alkaline conditions. Moreover, the UP-RuNi SAs /C allows an anion exchange membrane (AEM) electrolyzer to operate stably at 1.95 V cell for 250 h at 1 A cm −2 .

研究领域: 材料科学 · 电化学
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RENEWABLE ENERGY · 2025 · IF 9.1

Graphitic carbon nitride electronic structure evolution caused by niacin-derived carbon bridging benefits for Na+ adsorption to enhance the photocatalytic H2 production from artificial seawater splitting

Yu Zhang,Runzhe Li,Jingde Luan,Longde Jiang,Wengang Liu,Zheng Yan,Yu Bai

Photocatalytic hydrogen evolution from seawater splitting was a sustainable energy technology, alleviating the overuse of limited freshwater resources. The exogenous carbon was successfully doped into the framework of graphite carbon nitride via ultrasonic peeling and secondary calcination, replacing the bridging N atoms within the heptazine skeleton. This approach effectively regulated the chemical structure of g-C 3 N 4 , and the photocatalytic hydrogen yield of as-prepared CN-NA45 in water reached 7.15 mmolg −1 h −1 . In artificial seawater, the hydrogen yield of CN-NA45 increased to 10.80 mmolg −1 h −1 , which was attributed to the larger specific surface area, reduced band gap and more negative band edge. The presence of bridging carbon facilitated the transfer of electrons from the heptazine ring to the region near the bridging position, enhancing the local delocalization of π electrons. In artificial seawater, the adsorption of Na + ions on the catalyst surface were superior to other ions, facilitating the electron enrichment and providing more electrons for the photocatalytic reduction reaction. This work provided an insight into the construction of photocatalytic materials for marine environmental applications and the impact of electrolyte ions on hydrogen evolution performance.

研究领域: 材料科学 · 能源化学
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

High-efficiency removal of tetracycline by carbon-bridge-doped g-C3N4/Fe3O4 magnetic heterogeneous catalyst through photo-Fenton process

Xiao Zhang,Bin Ren,Xi Li,Biming Liu,Shiwen Wang,Peng Yu,Yanhua Xu,Guoqiang Jiang

Carbon-bridge-modified malonamide (MLD)/g-C 3 N 4 (CN) was prepared by copolymerization of MLD with urea and melamine and loaded with Fe 3 O 4 for the high-efficiency removal of tetracycline (TC) in water under photo-Fenton. The prepared catalysts were characterized by SEM, TEM , N 2 adsorption–desorption analysis, XPS, XRD, and FTIR, which proved that the modification method successfully introduced the C bridge into the carbon nitride molecular system and increased the structural defects of the catalyst. The Carbon-bridge-modified MLD/CN/Fe 3 O 4 also had good visible-light response and charge-separation and transport abilities in the photoelectrochemical test. Degradation results showed that the photo-Fenton degradation of TC reached 95.8%, and the mineralization rate was 55.7% within 80 min at 80 mM H 2 O 2 dosage, 0.5 g/L catalyst dosage, and near-neutral pH by 0.8MLD/CN/Fe 3 O 4 . Moreover, the oxidation products and mineralization pathways of TC were explored by LC-MS. Toxicity analysis indicated low environmental threat of the intermediates in TC mineralization. EPR analysis and H 2 O 2 decomposition efficiency analyses showed an improvement in the H 2 O 2 decomposition performance of 0.8MLD/CN/Fe 3 O 4 . This work could provide a valuable insight for the application of heterogeneous photo-Fenton technology in wastewater treatment .

CAS / MDL: 106-51-4 108-78-1
研究领域: 环境科学 · 化学工程 · 材料科学 · 水处理技术
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Atomic Ordered Array and Vacancy Defect Codependences of Electromagnetic Response in Nanocarbon Bridged-MXene Superlattices Absorbers

Zhongyan Gu,Ning Liu,Yudong Cheng,Yongpeng Wu,Chunhua Sun,Pengxu Chen,Fei Pan,Xiang Li,Wei Lu

Binary nanocrystals superlattices with the atomic long range ordered array of different colloidal nanocrystals are deemed as potential electromagnetic wave absorption (EWA) materials in dealing with current electromagnetic radiation problem, as their inherent superiority stems from the cooperative effect of adjacent units and strong interfacial coupling. However, relevant researches remain underdeveloped due to daunting synthetic challenges and complex electromagnetic regulation mechanism. Here, nanocarbon-bridged 2D-2D MXene superlattice with tunable vacancy defects are prepared via molecular ligands induced self-assembly and subsequently nitrogen-doped pyrolysis strategy, which resulted in “carbon-MXene-carbon-rGO-carbon” architecture. Such a periodic ordered & nano-bridging structure optimize axial charges transport over Van der Waals gap and suppressed interface formation between identical components, thereby boosting the charges localization and delocalization. Meanwhile, nitrogen doping further induce abundant Ti atom and Ti sub-nm clusters vacancy defects, together with generation of diverse dipole polarization centers. The synergistic effects of two mechanisms enabled programmable regulation of sum (ε'+ε'') and quotient (ε''/ε') of permittivity into predicted window required for low matching thickness, resulting in predictable EWA performance (1.5 mm, −56.3 dB). This work provides a versatile strategy for fabrication of atomic long range ordered heterostructures, paving the way for the development of absorbers via structural rearrangement and surface modification.

研究领域: 材料科学 · 纳米技术 · 电磁学 · 凝聚态物理 · 化学合成
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Dual Z-scheme 2D/3D carbon-bridging modified g-C3N4/BiOI-Bi2O3 composite photocatalysts for effective boosting visible-light-driven photocatalytic performance

Tongtong Zhang,Yuqi Wang,Xin Xie,Yanning Shao,Yuhao Zeng,Siyu Zhang,Qishe Yan,Zhongjun Li

A dual Z-scheme carbon-bridged g-C 3 N 4 /BiOI-Bi 2 O 3 photocatalyst were synthesized by simple solvothermal and calcination methods. The physical and chemical properties of prepared samples were explored via a series of characterization and Density Functional Theory (DFT) calculations. The formation mechanism of the composite photocatalyst was systematically studied and the formation process was simulated. Under the irradiation of visible light, 10% carbon-bridged g-C 3 N 4 /BiOI-Bi 2 O 3 exhibited the best photocatalytic performance. And the kinetics reaction model was followed pseudo-first-order kinetics. Moreover, the possible TC degradation pathways were established based on LC-MS. The enhanced photocatalytic activity was mainly attributed to the dual Z-scheme heterojunction formed by carbon-bridged g-C 3 N 4 deposition on the surface of Bi 2 O 3 and BiOI and a higher charge transfer rate of carbon-bridged g-C 3 N 4 , which effectively promoted the separation and transfer of electron-hole pairs. The trapping experiments were carried out to further explore its photocatalytic mechanism. This work provided an in-depth understanding of g-C 3 N 4 and bismuth-based catalysts.

研究领域: 材料科学 · 光催化 · 环境科学 · 化学
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