ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Fenglong Sun,Qian Jing,Tongda Xing,Yue Li,Bolong Jiang,Yang Zhao,Huan Wang
In this study, a Ag/CCN composite photocatalyst with a dragon-fruit section structure synthesized by loading silver nanoparticles (Ag NPs) onto CCN (g-C3N4 modified by M-phenylenediamine), is successfully employed as the photoanode in the H2O2 fuel cell system. Through the optimization of Ag NP loading amount, the 5%-Ag/CCN composite-based fuel cell exhibits a maximum power density of 1.195 mW·cm–2 in an aqueous solution containing 0.1 M HCl under AM 1.5G illumination (1 sun, 100 mW·cm–2), which is about 2.4 times higher than that of the g-C3N4-based fuel cell. The solar-to-electricity conversion efficiency (SECE) of the above fuel cell is further calculated to be 0.886%. Additionally, the 5%-Ag/CCN-based photocatalytic H2O2 fuel cell shows high stability during the charge and discharge process and strong energy storage capacity, along with a specific capacitance of 6860 mF·cm–2 after 2 h of irradiation and a capacitance retention rate of 60.33% even after 6 h of continuous operation. The localized surface plasmon resonance (LSPR) effect of Ag NPs significantly enhances the light capture capability of the photoanode, and the Schottky junction formed at the interface between Ag NPs and CCN effectively suppresses the recombination of photogenerated electrons and holes, promoting the photocatalytic oxidation of H2O to generate H2O2. This study provides a feasible strategy for constructing an efficient photoanode to generate H2O2, further improving the energy conversion efficiency and stability of H2O2 fuel cells.
研究领域:
材料科学
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能源科学
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光化学
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DOI
高影响因子
Sustainability
·
2025
·Vol. 17
·期 6
·2469
·
IF 3.3
Huidong Tang,Jiacheng Bao,Chen Liu,Yuwen Deng,Yixing Ma,Lei Shi,Shuangyou Bao,Kai Li,Ping Ning,Xin Sun
In pursuing sustainable environmental solutions, the concept of ‘waste to treasure’ has emerged as a promising approach. In this study, a new process is proposed to combine solid copper slag with hydrogen peroxide (H2O2) to remove nitrogen oxides (NOx) from acidic exhaust gases, thus effectively utilizing waste materials. Firstly, different smelting slags were screened to determine the catalytic potential of copper slag for hydrogen peroxide. Subsequently, the catalytic activity of the copper slags at various stages of the copper smelting process was thoroughly evaluated and optimized. In addition, a multifactorial evaluation of slow-cooled copper slag catalysts for removing NOx was carried out. Preliminary indications are that the iron phase in the copper slag is identified as the main source of catalytic activity sites. The results suggest that Fe2+/Fe3+sites on the surface of the Fe phase in the slow-cooled copper slag may be crucial in improving the NOx removal efficiency. The main reactive oxygen species detected in the system were ·OH, ·O2⁻, and1O2. In addition, the transformation products, formation pathways, and reaction mechanisms of NO in the liquid phase were initially investigated and determined. This study provides a green and sustainable path for the utilization of solid waste and management of atmospheric fumes in the non-ferrous metal industry and offers new perspectives to address environmental challenges in industrial processes.
研究领域:
环境科学
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冶金工程
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化学工程
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Shouhui Yi,Rongqiang Liao,Wei Zhao,Zuojin Liu
Stimulus-responsive nanomaterials , particularly with targeting capabilities, have garnered significant attention in the cancer therapy. However, the biological safety of these innovative materials in vivo remains unknown, posing a hurdle to their clinical application. Here, a pH/H 2 O 2 dual-responsive and targeting nano carrier system (NCS) was developed using core shell structure of Fe 3 O 4 mesoporous silicon (MSN@Fe 3 O 4 ) as main body, scutellarin (SCU) as antitumor drug and polymer cyclodextrin (PCD) as molecular switch (denoted as PCD@SCU@MSN@Fe 3 O 4 , abbreviated as NCS). The NCS, with an average particle size of 100 nm, displayed exceptional SCU loading capacity, a result of its uniform radial channel structure. The in vitro investigation under condition of pH and H 2 O 2 indicated that NCS performed excellent pH/H 2 O 2 -triggered SCU release behavior. The NCS displayed a higher cytotoxicity against tumor cells (Huh7 and HCT116) due to its pH/H 2 O 2 dual-triggered responsiveness, while the PCD@MSN@Fe 3 O 4 demonstrated lower cytotoxicity for both Huh7 and HCT116 cells. In vivo therapeutic evaluation of NCS indicates significant inhibition of tumor growth in mouse subcutaneous tumor models, with no apparent side-effects detected. The NCS not only enhances the bioavailability of SCU, but also utilizes magnetic targeting technology to deliver SCU accurately to tumor sites. These findings underscore the substantial clinical application potential of NCS.
研究领域:
药学
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生物医学工程
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肿瘤学
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产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
·
IF 19
Yimu Jiao,Qiyu Lian,Zhi Li,Muke Lin,Dingren Ma,Zhuoyun Tang,Dehua Xia,Mingshan Zhu
The p orbital electrons in main-group metals are generally underrated in the catalytic activity. Herein, an antimony (Sb) single-atom bipyridine-based covalent organic framework (SASb-TpBpy-COF) with the Sb─N coordination is successfully synthesized via 5p-2p orbitals hybridizarion for accomplishing the highly selective piezosynthesis of hydrogen peroxide (H 2 O 2 ) by the non-radical oxygen reduction reaction (ORR). Notably, the synthesized SASb-TpBpy-COF achieved an impressive H 2 O 2 piezosynthesis yield of 1500.58 µmol g −1 h −1 , which is up to more than 7-times higher than the reported catalysts. Moreover, the characterization results confirmed that the 5p-2p orbitals hybrid Sb single-atom can intrinsically drive the local polarization level, charge migration dynamics, electron-hole pairs separation, and affinity toward O 2 , consequently enhancing the piezoactivity and selective Pauling-type O 2 adsorption. Besides, experimental results clarified that the fast H 2 O 2 piezosynthesis is selectively dominated by the non-radical ORR. Furthermore, the dynamic Sb-OOH* intermediate is directly detected, proving the selective Pauling-type O 2 adsorption on the Sb single-atom sites. Moreover, this system can achieve an in situ degradation efficiency of over 80% for various emerging pollutants even in the real water samples. Conclusively, this study broadens the fundamental understanding for the fast H 2 O 2 piezosynthesis and provides a highly potential candidate technology for in situ water purification.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
Science Advances
·
2024
·Vol. 10
·期 16
·
IF 11.7
Zherui Zhang,Yuhao Luo,Yuanhong Ma,Yaofeng Zhou,Dingcheng Zhu,Wanhua Shen,Junqiu Liu
The in situ generation of H2O2 in cells in response to external stimulation has exceptional advantages in modulating intracellular Ca2+ dynamics, including high controllability and biological safety, but has been rarely explored. Here, we develop photocatalyst-based metal-organic frameworks (DCSA-MOFs) to modulate Ca2+ responses in cells, multicellular spheroids, and organs. By virtue of the efficient photocatalytic oxygen reduction to H2O2 without sacrificial agents, photoexcited DCSA-MOFs can rapidly trigger Ca2+ outflow from the endoplasmic reticulum with single-cell precision in a repeatable and controllable manner, enabling the propagation of intercellular Ca2+ waves (ICW) over long distances in two-dimensional and three-dimensional cell cultures. After photoexcitation, ICWs induced by DCSA-MOFs can activate neural activities in the optical tectum of tadpoles and thighs of spinal frogs, eliciting the corresponding motor behaviors. Our study offers a versatile optical nongenetic modulation technique that enables remote, repeatable, and controlled manipulation of cellular and animal behaviors.
研究领域:
细胞生物学
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生物医学工程
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神经科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
·
IF 11.2
Shuang Zhou,Da Wen,Wei Zhong,Jianjun Zhang,Yaorong Su,Aiyun Meng
The effective adsorption of oxygen (O 2 ) molecules over photocatalysts is a critical step in promoting the performance of photocatalytic H 2 O 2 production. However, g-C 3 N 4 usually features a Yeager-type (side-on) adsorption configuration of O 2 molecules, which causes the breaking of O–O bonds and severely hinders the H 2 O 2 production activity. Herein, we synthesized an oxygen-vacancy-rich TiO 2– x /g-C 3 N 4 step-scheme (S-scheme) heterojunction to regulate the oxygen adsorption configuration and improve the 2e – ORR selectivity of H 2 O 2 production. In-situ X-ray photoelectron spectroscopy (in-situ XPS) and density functional theory (DFT) calculations reveal that the S-scheme heterojunction is formed between TiO 2– x and g-C 3 N 4 . The difference between their Fermi levels leads to the electron flow from g-C 3 N 4 to TiO 2– x , which increases the electron-deficient sites in g-C 3 N 4 . As a result, the cleavage of O–O bonds on the surface of g-C 3 N 4 is avoided and the oxygen adsorption configuration is tuned from Yeager-type to Pauling-type (end-on). Consequently, the photocatalytic H 2 O 2 production rate is dramatically improved to 1780.3 μmol h –1 , which is about 5 times higher than that of pristine g-C 3 N 4 . This work paves a new way to tailor the oxygen adsorption configuration by rationally designing S-scheme heterojunction photocatalysts.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2024
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IF 11.3
Ruilin Liu,Chao Wang,Yong Yan,Ruzhi Wang,Ge Chen
The direct hydrogen peroxide (H2O2) product from H2 and O2 is a promising anthraquinone replacement because it is environmentally friendly and has a high atom efficiency. Experimental and theoretical studies have proven that optimizing the adsorption of the critical intermediate OOH* on the metal site significantly promotes the further protonation of this intermediate and inhibits the O–O bond cleavage, thus enhancing the activity and selectivity. Redistributing the charge density of active sites to tuning the d-band center of the metal could effectively modulate the intermediates adsorption, and thus regulate the catalytic efficiency. Herein, we show that a Lewis acid (ZnCl2 solution) induces abundant oxygen vacancies (Ovs) on the TiO2 surface, which results in a reversal of charge transfer from TiO2–Ov support to the Pd atom, generating an electron-rich Pd configuration. Compared with pristine Pd/TiO2, Pd/TiO2–Ov possesses higher H2O2 selectivity and productivity, with values of 80.7% and 186 mol kgcat–1 h–1, respectively. In addition, Pd/TiO2–Ov maintains stability during the six cycles reaction due to its high resistance to the leaching of Pd species. Theoretical calculations reveal that the reversed charge transfer downshifts the d-band center of Pd, which promotes O2 adsorption on the Pd surface and weakens the OOH* intermediates adsorption. Thus, the energy barrier for the hydrogenation of the OOH* intermediate is significantly decreased, and the O–O band cleavage is inhibited. This study reports a reversal of charge transfer tuning the d-band center of the active site for efficient direct H2O2 synthesis, which may provide insight for designing high-performance catalysts.
研究领域:
化学
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材料科学
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催化
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环境科学
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产品关联
DOI
高影响因子
Applied Sciences-Basel
·
2025
·Vol. 15
·期 11
·5945
·
IF 2.5
Lia Wang,Xu He,Lan Liang,Yanshan Wang,Beibei Yan,Guanyi Chen,Ning Li,Li’an Hou
The conventional Fenton process generates large amounts of Fenton sludge during wastewater treatment. Achieving effective utilization of Fenton sludge and reducing its production remain pivotal challenges. In this study, Fenton sludge biochar catalysts (Cat) were prepared using Fenton sludge via pyrolysis. In addition, chemical oxygen demand (COD) from secondary effluent was removed by Fenton sludge biochar catalysts activated with H2O2/Fe(VI). Specifically, the removal efficiency of COD could reach 46.2% in the Cat−2/H2O2/Fe(VI) system under weakly alkaline conditions. The mechanistic analysis confirmed that high-valent iron,•OH, O2•−, and1O2all participate in the degradation process. Furthermore, a continuous-flow reactor was applied to treat secondary effluent, with COD decreasing from 65 mg/L to 36 mg/L. This study provides new insights into the resource utilization of Fenton sludge and the treatment of complex wastewater.
研究领域:
环境科学
·
废水处理
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Peiyang Gu,Feiyang Tan,Wuzi Zhao,Jingwen Dong,Shiyuan Zhou,Xiaoqiong Hao,Shengsheng Gu,Guangfeng Liu,Danfeng Wang
Photocatalysis has unprecedently prevailed in the removal of pollutants and the artificial photosynthesis of H 2 O 2. However, inefficient surface reaction and exciton dissociation rate are the main hurdles in arriving at high photocatalytic performance. A versatile strategy for improving surface reactions between the photocatalyst and the reactant and the charge separation dynamics is in pressing need. Herein, post-quaternization of the conjugated microporous polymer (CMP) is proposed. This not only converts the CMP from hydrophobic to hydrophilic but also evidently improves charge separation and mobility due to the polarizing effect. Most importantly, because of the quaternization, the surface reactions can be pronouncedly strengthened due to both the improved dispersity and lowering of O 2 adsorption energy. As a result, the CMPs serve both photodegradation and photosynthesis of H 2 O 2 , with iB-TDZ exhibiting pronounced enhancement in the photodegradation of 100 ppm of Congo red and 2,4-D in 40 min and 90 min, respectively, transcending the vast majority of the reported photocatalysts, while the production of H 2 O 2 reaches 2.922 mmol g −1 in three-hour irradiation. As a proof-of-concept experiment, simultaneous photodegradation of 2,4-D and photocatalytic H 2 O 2 production is realized. It was found that 2,4-D can boost photocatalytic H 2 O 2 production from 1.92 mmol g −1 (without 2,4-D) to 3.25 mmol g −1 within 90 min, likely due to its role in providing protons and serving as an h + scavenger. These findings provide a fresh platform for the design of CMP-based photocatalysts for simultaneous photocatalytic wastewater treatment and H 2 O 2 production.
研究领域:
环境科学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Dingliang Dai,Jianhao Qiu,Guanglu Xia,Yong Tang,Qiying Liu,Yixin Li,Biyao Fang,Jianfeng Yao
Metal-organic framework derived materials received a lot of attention due to their significant benefits in photocatalytic reactions. In this work, a Z-scheme ZnIn 2 S 4 /Bi 2 S 3 hierarchical heterojunction is first developed by a one-pot method using CAU-17 as a template. The specific preparation method endows an intimate interface contact between these two monomers, and CAU-17-derived Bi 2 S 3 possesses a high surface area and porosity, resulting in an efficient charge separation and O 2 capture. Thus, for photocatalytic H 2 O 2 production from the O 2 reduction reaction, the ZnIn 2 S 4 /Bi 2 S 3 heterojunction can achieve an H 2 O 2 yield of 995 µmol L −1 in pure water and ambient air under visible light, 4.5 and 4 times that of ZnIn 2 S 4 and Bi 2 S 3 , respectively. In addition, in tetracycline solution, ZnIn 2 S 4 /Bi 2 S 3 can degrade tetracycline with a degradation rate of 95% by photocatalysis, and at the same time, a final H 2 O 2 production yield of 1223 µmol L −1 is reached. Similarly, high yields of H 2 O 2 are also obtained from wastewater containing o -nitrophenol, acid golden yellow, or acid red, and these pollutants are effectively degraded. This work reveals the potential of metal-organic framework-derived materials in photocatalysis, as well as provides insights into H 2 O 2 green synthesis and wastewater treatment.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Mengran Liu,Canyu Liu,Tianfang Yang,Shixiang Hu,Siyun Li,Shizhe Liu,Yang Liu,Ye Chen,Bingcheng Ge,Shuyan Gao
Transition metal Ni anchored in carbon material represents outstanding 2e − oxygen reduction reaction (ORR) catalytic selectivity, but enhancing the adsorption strength of intermediate *OOH to promote its selectivity remains a major challenge. Herein, the NiX/Ni@NCHS composite catalyst with heteroatom doping (O,S) is modulated by controlling partial pyrolysis strategies on honeycomb-like porous carbon to manipulate the electronic structure of the metal Ni. With the synergistic effect of honeycomb structure and O atom, NiO/Ni@NCHS-700 exhibits an exceptional H 2 O 2 selectivity of above 89.1% across a wide potential range from 0.1 to 0.6 V in an alkaline electrolyte, and an unexpected H 2 O 2 production rate up to 1.47 mol g cat ‒1 h ‒1 @0.2 V, which outperforms most of the state-of-the-art catalyst. Meanwhile, NiS/Ni@NCHS exhibits excellent electrocatalytic performance, with 2e − ORR selectivity of 91.3%, H 2 O 2 yield of 1.85 @0.3 V. Density functional theory simulations and experiments results reveal that the heteroatom doping (O,S) method has been employed to regulate the adsorption strength of Ni atoms with *OOH, and combined with the self-sacrificing template-assisted pyrolysis approach to improve the microstructure of catalysts and optimize the active site. The heteroatom doping method in this work provides significant guidance for promoting 2e − ORR electrocatalysis to produce H 2 O 2 .
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 10
·4823-4832
·
IF 3.5
Haihui Hu,Ke Ma,Yuandong Yang,Na Jin,Linjie Zhang,Jinjie Qian,Lili Han
Hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction (2e− ORR) represents a green alternative to the energy-intensive anthraquinone process. However, the practical application of this method is limited by the lack of cost-effective and high-performance electrocatalysts. Reported here is a hybrid catalyst composed of nickel (Ni) clusters immobilized onto the surface of two-dimensional siloxene nanosheets (Ni/siloxene), which exhibits excellent efficiency and selectivity in electrocatalytic oxygen reduction to H2O2 in an alkaline medium, demonstrating a standard 2e− pathway with >95% H2O2 selectivity across a wide potential range. Experimental results disclose that the high performance of Ni/siloxene can be traced to a synergy of the Ni clusters and the oxygen-rich surface of siloxene. Density functional theory (DFT) calculations further reveal a weakened interaction between Ni/siloxene and *OOH and the consequently reduced energy barrier for the *OOH protonation toward H2O2 desorption, thus leading to a high 2e− ORR reactivity and selectivity. This work provides a valuable and practical guidance for designing high-performance 2e− ORR electrocatalysts based on the rational engineering of the metal–support interaction.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）