KOREAN JOURNAL OF CHEMICAL ENGINEERING
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2016
·Vol. 33
·期 12
·3407-3416
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IF 1.408
Wu Bo,Xiong Yuanquan,Ru Jinbo,Feng Hao
A novel NO removal system is designed, where NO is initially oxidized by •OH radicals from the decomposition of hydrogen peroxide (H 2 O 2 ) over hematite and then absorbed by ammonium-based solution. According to the high performance liquid chromatography (HPLC) profile and the isopropanol injection experiments, the •OH radicals are proved to play a critical role in NO removal. The NO removal efficiency primarily depends on H 2 O 2 concentration, gas hourly space velocity (GHSV), H 2 O 2 feeding rate and reaction temperature, while the flue gas temperature slightly affects the NO removal efficiency. The low H 2 O 2 consumption makes this system a promising technique in NO removal process using wet-method. The evolution of catalyst in reaction is analyzed by scanning electron microscopy (SEM), energy dispersive X-ray spectrometry (EDS), Fourier Transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD). The nitrite ion and nitrate ion in aqueous solution are detected by the continuous phase flow analyzer. Finally, the macrokinetic parameters of the NO oxidation are obtained by using the initial rate method.
研究领域:
环境科学
·
化学工程
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Xingang Kong,Yanlei Li,Yue Zhang,Lifeng Zhang,Jianfeng Huang,Qi Feng
Usually, it takes 3–7 days to exfoliate the layered titanic acid H 1.07 Ti 1.73 O 4 (HTO) into Ti 1.73 O 4 1.07– (TO) nanosheet . The H 2 O 2 molecules can easily enter into the interlayers of the HTO crystal to form the H 2 O 2 intercalated HTO. The H 2 O 2 intercalation can achieve rapid exfoliation of HTO. It takes 1 h to exfoliate into a yellow H 2 O 2 -modified TO nanosheet, which has a wide absorption wavelength range and a narrow band gap. Moreover, such 2D nanosheet has a large specific surface area and a large number of reactive sites. And such yellow H 2 O 2 -modified TO nanosheet displays some visible photocatalytic hydrogen production performance. When the H 2 O 2 -TO nanosheet is loaded with Ni(OH) 2 , the sample can show a higher photocatalytic hydrogen production performance. The maximum photocatalytic hydrogen production rate of the Ni(OH) 2 -H 2 O 2 -TO catalyst is 32.48 μmol h −1 g −1 , which is 4.1 and 1.9 times higher than that of H 2 O 2 -TO and Pt-H 2 O 2 -TO. This is due to the formation of a type II heterojunction between the H 2 O 2 -TO nanosheet and Ni(OH) 2 . This heterojunction can achieve the effective separation of photogenerated carriers.
研究领域:
材料科学
·
光催化
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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
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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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DOI
高影响因子
Science Advances
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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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PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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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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PubMed
高影响因子
ACS Catalysis
·
2024
·
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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高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 10
·4823-4832
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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
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电化学
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催化
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纳米技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yuan Chang,Zhenzi Li,Shijie Wang,Xuepeng Wang,Bo Wang,Lijun Liao,Wei Zhou
Metal-deficient Zr nodes are constructed in UiO-66-NH 2 by vacuum treatment. • Zr-node microenvironment regulation enhances charge separation and O 2 activation. • UN 200/28 achieves 272.9 μmol g −1 h −1 H 2 O 2 production in pure water. • UN 200/28 delivers a 20-fold activity increase and 6.36% AQY at 420 nm. • H 2 O 2 formation follows an ORR-dominated pathway with secondary WOR contribution. Photocatalytic H 2 O 2 production from pure water and O 2 offers a sustainable route for green oxidant synthesis, yet its efficiency is limited by insufficient O 2 activation, sluggish charge separation, and poorly defined active sites. Herein, a metal-defect-engineered UiO-66-NH 2 photocatalyst is constructed through high-temperature vacuum treatment to regulate the Zr-node coordination microenvironment. The optimized UN 200/28 preserves the UiO-66-NH 2 crystalline framework and octahedral morphology, while a 7.8% decrease in Zr content is confirmed by ICP, STEM, FTIR, XPS and EPR, thereby indicating the formation of metal-deficient Zr nodes and the reconstruction of the local Zr O coordination microenvironment. These defect-induced structural modifications broaden visible-light absorption, narrow the band gap from 2.88 to 2.57 eV, and promote photogenerated charge separation and transfer. UN 200/28 exhibits markedly enhanced photocatalytic H 2 O 2 production in pure water under O 2 , achieving an H 2 O 2 formation rate of 272.9 μmol g −1 h −1 , a 20-fold improvement over pristine UiO-66-NH 2 , and an apparent quantum yield of 6.36% at 420 nm. The O 2 reduction and water oxidation processes account for approximately 63.2% and 36.8% of the total H 2 O 2 formation, respectively. This work demonstrates that cluster-level regulation of the Zr-node coordination microenvironment is an effective strategy for enhancing photocatalytic H 2 O 2 production in pure water. Download: Download high-res image (110KB) Download: Download full-size image
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PHYSICA B-CONDENSED MATTER
·
2026
·
IF 3.2
Junyu Huang,Di Lin,Wei Li,Bo Wang,Huiyang Xu,Zimo Wang,Yongyi Li,Shuanglong Li,Xiaorui Huang
The PCN/CdS/CdIn 2 S 4 composites exhibit excellent photocatalytic performance for H 2 evolution, H 2 O 2 production and dye degradation. • Spontaneous interfacial band bending drives a dual Z-scheme pathway to preserve highly active photogenerated charge carriers. • The superoxide radicals (.•O 2 − ) is the primary species for both continuous H 2 O 2 generation and rapid pollutant decomposition. Addressing the escalating global energy and environmental crises demands efficient, sustainable, and robust technologies. In this study, a ternary composite PCN/CdS/CdIn 2 S 4 integrating phosphorus-doped carbon nitride (PCN), cadmium sulfide (CdS), and indium cadmium sulfide (CdIn 2 S 4 ) was rationally designed via a multi-step assembly process. The optimized heterojunction exhibits outstanding performance, achieving remarkable H 2 and H 2 O 2 production rates of 7614 and 6873 μmol∙g −1 h −1 , respectively. Additionally, it demonstrates ultra-fast degradation kinetics, mineralizing 99.4% of methyl orange within just 30 min. Mechanistically, spontaneous interfacial band bending drives a dual Z-scheme charge transfer pathway. This specific energy band alignment effectively preserves strongly reducing electrons and highly oxidizing holes while significantly suppressing charge carrier recombination. Furthermore, radical trapping confirms that superoxide radicals (∙O 2 − ) are the pivotal active species, driving a two-step single-electron reduction pathway (O 2 →∙O 2- →H 2 O 2 ) for continuous H 2 O 2 generation, and coupling synergistically with localized holes for rapid organic pollutant decomposition.
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ACS Catalysis
·
2026
·Vol. 16
·期 15
·14932-14942
·
IF 13.6
Liu Mengxin,Zhang Pu,Chen Boran,Yang Zhenyu,Che Huinan,Ao Yanhui
Dark photocatalysis decouples light harvesting from catalysis via photogenerated charge storage, enabling H 2 O 2 production under intermittent illumination. However, increasing electron-storage capacity alone does not ensure efficient dark-state H 2 O 2 production, and how stored electronic states influence oxygen reduction reaction (ORR) remains unclear. Here, we show that polaron delocalization contributes to multi-electron ORR selectivity in poly(heptazine imide) (PHI), allowing dark photocatalytic H 2 O 2 synthesis. Sulfonated PHI (S-HPHI) delivers a 2.5-fold higher H 2 O 2 yield (588.9 μmol g –1 ) than protonated PHI (HPHI, 237.3 μmol g –1 ) despite comparable net photo-contributed electron-storage capacities (1441–1752 μmol e – g –1 ). This enhancement is consistent with the higher electron utilization efficiency toward H 2 O 2 formation (81.7% for S-HPHI versus 27.1% for HPHI), enabled by sulfonation-induced polaron delocalization. Combined experimental and theoretical analyses reveal that sulfonation promotes polaron delocalization and disperses structural relaxation during photocharging. These changes are consistent with reduced electron self-trapping and facilitated directional electron transfer to adsorbed O 2 , which may contribute to suppressing O–O bond cleavage in proton-coupled electron transfer steps. This favors enhanced selectivity toward H 2 O 2 formation even at high stored-electron densities. These findings highlight polaron delocalization as an important factor contributing to improved reaction selectivity in dark photocatalysis.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Ningchao Zheng,Zhizeng Pan,Shuai Kang,Deqian Zeng,Xiangbiao Yin,Qiang Wu,Yuezhou Wei,Zhuofeng Hu
Hydrogen peroxide (H 2 O 2 ) is regarded as a promising strategy for radioactive uranium removal, due to its eco-friendliness and ability to convert free UO 2 2+ into insoluble studtite. However, the spontaneous and selective production of H 2 O 2 under ambient conditions remains challenging. This study develops a P-Ag for spontaneous O 2 activation and selective H 2 O 2 synthesis under ambient conditions. The H 2 O 2 yields of P-Ag reach 1210 µmol g −1 h −1 in air and 1876.3 µmol g −1 h −1 in O 2 , surpassing most of the recently reported catalytic systems. Importantly, the H 2 O 2 generated in situ by P-Ag achieves a high uranium removal activity (48.5) within 60 min, outperforming 23 known systems. Mechanistic studies indicate that P-Ag follows a two-step single-electron O 2 activation pathway. The electron-donating Ag sites drive the complete catalytic cycle, encompassing H 2 O/O 2 adsorption, H 2 O dissociation, and *OOH/H 2 O 2 formation, while the red phosphorus substrate serves as an electron reservoir to sustain the Ag sites. The H 2 O 2 produced reacts instantaneously with UO 2 2+ to form studtite, enabling efficient uranium removal. This study not only offers new insights into the selective synthesis of H 2 O 2 via spontaneous O 2 activation, but also proposes an eco-friendly route to mitigate environmental risks from radioactive uranium contamination.
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高影响因子
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