JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Wang Lv,Shangkai Qiu,Lu Xiong,Zhiyong Yan,Hou Wang,Yan Wu
Mo 4d-S 3p orbital hybridization effectively reshapes the electronic band structure. • Sulfur vacancies shift from recombination centers to efficient charge-transfer channels. • Mo S Ni bridging orbital channels establish a robust built-in electric field. • Mo–Ni orbital synergy enables a highly selective 2e⁻ oxygen reduction pathway. This work addresses the fundamental dilemma between charge separation efficiency and surface reaction selectivity in heterogeneous photocatalysis through synergistic orbital engineering. By introducing Mo dopants and sulfur vacancies (V S ) into Zn 3 In 2 S 6 , the localized electronic states of isolated V S are transformed into delocalized charge channels via strong Mo 4d-S 3p orbital hybridization. This orbital-level modulation effectively suppresses charge recombination while optimizing the band structure for visible-light absorption. Coupled with in-situ grown Ni 4 S 3 , an interfacial Mo-S-Ni orbital bridge is constructed, which not only establishes a robust built-in electric field to direct electron flow toward Ni 4 S 3 but also tailors the local coordination environment for selective two-electron oxygen reduction. The resulting heterojunction photocatalyst achieves an exceptional H 2 O 2 production rate of 163.0 ± 2.1 μM h −1 in pure water without any sacrificial agent. Notably, the H 2 O 2 production rate of 252.1 ± 2.4 μM h −1 is attained at a tetracycline hydrochloride (TC) concentration of 20 mg L −1 , 1.5 times higher than that in pure water. This study demonstrates that precise orbital coupling can integrate carrier dynamics management with reaction pathway control, providing a new design paradigm for noble metal-free, high-performance and multifunctional photocatalytic systems. Download: Download high-res image (216KB) Download: Download full-size image
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高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Zhouling Wu,Zhixuan Zhang,Zhiqi Liang,Li Cheng,Shuang Yang,Zhengxing Jiang,Yurong Qi,Zufei Hu,Yang Yang
Crystal plane engineering is an emerging strategy for enhancing the surface activity of catalysts, but there is little research on how crystal planes affect electrochemical non-enzymatic H 2 O 2 sensors. We synthesize four distinct NiCo 2 O 4 nanocrystals with different crystal planes and investigate their impact on electrochemical non-enzymatic H 2 O 2 sensing through a systematic combination of experimental and theoretical approaches. NiCo 2 O 4 nanosheets exposing the {3 1 1} crystal plane (311-NS) demonstrate the highest electrocatalytic activity for H 2 O 2 oxidation, with excellent selectivity, repeatability, reproducibility, and long-term stability. The H 2 O 2 detection performance of NiCo 2 O 4 with is consistent with the total amount of surface Co 3+ and Ni 3+ , indicating that the Co 3+ and Ni 3+ exhibit higher activity for H 2 O 2 oxidation. Our density functional theory calculations attribute the superior sensing performance of 311-NS primarily to its high dangling bond density of Co(III) and Ni(III) and its increased surface energy, both facilitate the oxidation of H 2 O 2 . We additionally construct a 311-NS/rotating disk electrode sensor that detects H 2 O 2 in real samples with accuracy comparable to that of high-performance liquid chromatography, highlighting its potential for applications in environmental monitoring and food safety. This study not only broadens our understanding but also demonstrates that selective exposure of specific crystal planes enhances electrochemical non-enzymatic H 2 O 2 sensing performance, an insight to guide development of future peroxide sensors.
研究领域:
材料科学
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电化学
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传感器技术
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ACS Nano
·
2025
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IF 16
Yingbi Chen,Qingguo Feng,Yu Bai,Meng Wang,Yuchao Wang,Peiyao Yang,Danni Deng,Xinran Zheng,Jiabi Jiang,Haitao Zheng,Guozhao Fang,Yi Zeng,Xiang Xiong,Yongpeng Lei
Electrochemical two-electron oxygen reduction reaction (2e– ORR) to produce hydrogen peroxide (H2O2) is attractive, but poor H2O2 selectivity and activity need to be overcome. Herein, a phosphorus-induced electron pump is demonstrated. The H2O2 selectivity reaches >90% (93.5% at 0.5 V) in the potential range of 0.2∼0.7 V. The Faradaic efficiency achieves 94.2% at 0.6 V. In situ Raman experiment and density functional theory calculation indicate that the O2 adsorption and activation are enhanced. The *OOH intermediates are formed at a more positive potential. Furthermore, the universal mechanism of the electron pump is extended. At last, the potential to degrade antibiotics, Escherichia coli, etc., on site is confirmed. This work displays that the phosphorus-induced electron pump activates O2, which provides an insight into the electrocatalytic 2e– ORR.
研究领域:
电化学
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催化
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材料科学
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环境科学
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化学工程
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JOURNAL OF CATALYSIS
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2024
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IF 6.5
Lei Wu,Ruiting Xue,Yang Li,Shaobo Cao,Jian yang,Ximei Fan
Metal/semiconductor heterostructures have been widely used to drive photochemical reactions. However, understanding of the synergies between them is still limited. In this study, we discovered that under ultraviolet (UV) light, rather than visible (Vis) excitation, the redox active sites oxidize adsorbed water and reduce oxygen molecules more efficiently. In this paper, the comprehensive mechanism of Ag@TiO 2 photocatalysis of H 2 O 2 has been elucidated and confirmed their synergies in photocatalytic reactions, through in situ characterization and theoretical calculation. Our findings provide insights into the key factors that influence the difference of photoactivity in UV and Vis light, thus having important implications for the design of solar energy conversion materials as well as environmental purification materials.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shujun Sun,Jun Zhang,Changdong Sheng,Hui Zhong
NO in flue gas is one of the atmospheric pollutants, and it is necessary to study effective NO removal technology. It was identified that the alkaline H 2 O 2 system achieved over 98 % NO removal efficiency with a gas–liquid contact time of 3 s in this paper. This paper investigates the mechanism of NO removal in alkaline H 2 O 2 solution through both experimental and theoretical calculations. The results reveal the NO removal process can be divided into three phases by the NaOH/H 2 O 2 molar ratio. (1) The ∙O 2 – dominated phase, where trace metal Fe catalyzes ∙O 2 – radical generation from H 2 O 2 as Fe (OH) 2+ , reacting primarily with NO to form ONOO – . The energy barrier for this process is1.299 kcal/mol, with a reaction rate constant of 9.12 E + 11 s -1 M −1 . (2) The HO 2 – dominated phase, HO 2 – was generated through OH – and H 2 O 2 neutralization, which converts NO to NO 2 and regenerating OH – . The energy barrier for HO 2 – reacting with NO is 3.833 kcal/mol, and the reaction rate constant is 2.07E + 10 s -1 M −1 . (3) The O 2 2– dominated phase, O 2 2– was a further ionization of HO 2 – and converting NO to NO 2 – directly. The energy barrier for this process is 7.079 kcal/mol, and the reaction rate constant is 1.49 E + 08 s -1 M −1 .
研究领域:
环境科学
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化学工程
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-8
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IF 15.7
Hu Yunhao,Yang Weifeng,Ma Yuji,Qiu Yong,Wei Wei,Wu Bo,Li Kerui,Li Yaogang,Zhang Qinghong,Xiao Ru,Hou Chengyi,Wang Hongzhi
Solid-liquid contact electrification is a widespread interface phenomenon in nature. Recent research and theory demonstrate that electron transfer during this process holds the potential to initiate interfacial chemical reactions. Here, we design a dual-functional device for generation of H 2 O 2 and energy. Interfacial chemical reactions and solid-liquid contact charging occur simultaneously during the liquid phase flow process. Specifically, electron transfer at the solid-liquid interface induces the formation of hydroxyl radicals (·OH) in the liquid phase, leading to spontaneous generation of H 2 O 2 . The transfer of charges at the solid-liquid interface is accompanied by energy transfer. By designing an external electrode structure, we can effectively harvest the energy from the flowing liquid phase, yielding an output power of up to 5.8 kW/m 3 for water.
研究领域:
材料科学
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化学工程
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能源科学
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高影响因子
ACS ES&T Water
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2024
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IF 4.8
Yuxin Shi,Qiong Zhu,Lanlan Fu,Jixing Wang,Xinyan Lu,Ying Tao,Chi Zhang,Yongjie Wang,Kangning Xu,Huan Shang,Dieqing Zhang,Guisheng Li
The solar-powered photocatalytic oxygen reduction reaction is considered a promising alternative method for H2O2 production under mild reaction conditions. However, the intrinsic competitive pathway grossly inhibits the selectivity and final yield of H2O2 accompanying the loss of photogenerated electrons during the oxygen reduction reaction process. Herein, two-coordinate nitrogen (N2C) vacancy-rich g-C3N4 (DCN1.2) was developed by polymerization pyrolysis using the bottom-up strategy. DCN1.2 with a low-coordinated N2C-vacancy enabled an enhanced H2O2 production in a wide pH range. The optimized DCN1.2 demonstrated a H2O2 yield of 556.2 μmol·gcat–1·h–1 at pH = 10, which was approximately 3 times higher than that of pristine CN (202.7 μmol gcat–1·h–1). DFT calculations and photochemical experimental results revealed that N2C-vacancies induced the asymmetric electron distribution of DCN, thereby facilitating electron transfer and promoting the O2 adsorption/activation for H2O2 production. Additionally, EPR and situ FTIR measurements indicated that DCN1.2 could produce H2O2 via a sequential two-step single-electron pathway, thereby achieving efficient H2O2 production with good selectivity. This study provides guidance for the rational design of defect-engineering g-C3N4 catalysts for efficient photocatalytic H2O2 generation.
研究领域:
材料科学
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环境科学
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化学工程
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Quanhua Xie,Xiaoyu Zhong,Yang Liu,Wenliang Fan,Yuanyuan He,Yuan Zhou,Xuefeng He,Zhenting Xie,Yejun Xiao,Nianbing Zhong
To achieve online, rapid, selective, and accurate detection of H 2 O 2 in UV/H 2 O 2 -based photo-oxidative processes for optimizing ⋅OH production, this study developed a long-period fiber grating (LPFG)-based H 2 O 2 sensor using a graphene oxide (GO)-loaded two-line ferrihydrite (2L-Fht) nanozyme. The GO/2L-Fht sensing layer was synthesized via surface precipitation and immobilized onto the grating surface through a combination of chemical bonding and physical adsorption techniques. Acting as a peroxidase-like nanozyme with high enzymatic activity over a wide pH range, 2L-Fht catalyzes the decomposition of H 2 O 2 , releasing water molecules. GO interacts with these water molecules, altering its effective refractive index and inducing a resonance wavelength shift in the LPFG transmission spectrum. The H 2 O 2 concentration was determined by monitoring the wavelength shift. The effects of doping content, coating thickness, and the pH of the solution on sensor performance were investigated. The results demonstrated at a 2L-Fht doping content of 25 wt%, a coating thickness of 958 nm, and a pH of 7.0, the sensor achieved sensitivities of 95.18 and 285 pm/lg( c ) for H 2 O 2 concentration ranges of 10⁻ 8 to 10⁻ 2 M and 0.01 to 1 M, respectively. Additionally, it exhibited a detection limit as low as 3.99 nM and a response time of 6–14 s. The sensor also exhibited high selectivity and repeatability. This study presents the first use of GO/2L-Fht composites for H 2 O 2 sensing, offering an effective approach for rapid and sensitive detection across a pH range of 5–9 and broadening the applications of fiber optic sensing technology.
研究领域:
光学传感
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环境监测
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纳米材料
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化学传感器
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水处理技术
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高影响因子
Green Chemical Engineering
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2026
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IF 11.9
Chuan-Bin Li,Ling-Yu Dong,Yi-Fan Wang,Guang-Ping Hao
Electrosynthesis of hydrogen peroxide (eH 2 O 2 ) offers a facile and environmentally benign synthesis alternative through selective two-electron oxygen reduction reaction (2e – ORR). Carbon-based nonprecious electrocatalysts are promising for 2e – ORR, however, its efficiency is often limited by low intrinsic activity and limited accessibility of catalytic sites. Here, we present a family of carbonyl rich carbon spheres with surface wrinkle structure, which was engineered to boost the activity for 2e – ORR and to enlarge its electrochemical active surface area. As compared to common O-doped carbon spheres, our materials with controlled surface wrinkles delivered a 10-fold enhancement of accessible active surface area. Extensive catalytic tests together with characterizations indicate carbonyl moieties are the predominant active sites for O 2 activation. In 0.1 M KOH electrolyte, the catalyst delivered the H 2 O 2 selectivity of > 97.5% over a large potential range from 0-0.67 V vs . RHE, which resulted in a H 2 O 2 production rate of 385 mmol/(g·h) at 0 V vs. RHE. This study provides a useful surface structure fine modulation method for the development of heteroatom-doped carbon electrocatalysts for selective H 2 O 2 synthesis.
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Molecular Catalysis
·
2023
·
IF 4.6
Bin Wu,Xiangyun Wang,Bo Yang,Yunjian Ma,Frank Hollmann,Yonghua Wang
In the present work we propose a bienzymatic cascade for the oxyfunctionalisation of cycloalkanes to cyclic alcohols/cyclic ketones. By combining a H 2 O 2 -dependent peroxygenase with a O 2 -consuming and H 2 O 2 -producing alcohol oxidase an overall aerobic oxidation system was established. A convincing proof-of-concept is presented and some current limitations are outlined.
研究领域:
生物化学
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酶工程
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高影响因子
CATALYSIS COMMUNICATIONS
·
2016
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IF 3.389
Xiaomin Xiang,Bin Zhang,Guoqiang Ding,Jinglei Cui,Hongyan Zheng,Yulei Zhu
The oxidation of furfural in H 2 O 2 and H 2 O 2 –Mg(OH) 2 system were systematically investigated and a rational explanation for the reaction mechanism was proposed. 2-formyloxyfuran, from selective oxidation of HC O group in furfural, was a crucial intermediate. The addition of Mg(OH) 2 suppressed the oxidation of furan ring of furfural and enhanced selectivities of 2(5H)-furanone (44.8%) and succinic acid (38.0%). FT-IR, Gaussian calculation and experimental results indicated that the process of furfural oxidation with H 2 O 2 is homogeneous, and the synergy between dissolved Mg 2 + cations and OH − ions facilitates the HOO − attacking the carbon atom of HC O other than the C C bound of furan ring.
研究领域:
化学工程
·
催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Gang Wang,Jiayu Gao,Yike Fu,Zhaohui Ren,Jie Huang,Xiang Li,Gaorong Han
The anticancer efficacy of chemodynamic therapy (CDT) is considerably restrained by the inadequate content of H 2 O 2 within tumor microenvironment (TME), unexpected oxidation of Fenton agents and low targeting efficiency of particulate therapeutic platforms. Herein for the first time, an implantable CDT platform was designed and synthesized by combining Fe 0 nanocrystal embedded mesoporous silica nanoparticles (FeMSN) and PCL-gelatin fibres (PG fibres), denoted as [email protected] fibres. FeMSN was fabricated via in situ reduction of ferrous ions within the mesopores of MSNs, and assembled at the surface of electrospun PG fibres by electrostatic interaction to form a fibrous mesh. The findings reflected that, in an acid condition, FeMSN nanoparticles can liberate from the composite fibres, and be effectively uptaken by 4T1 cancer cells. The FeMSN released may react with oxygen to generate H 2 O 2 in the acidic microenvironment, and subsequently transform H 2 O 2 to intracellular hydroxyl radicals, inducing enhanced cell-killing effect. By implanting the composite fibres locally at the tumor site of mice, promoted anticancer efficacy was observed with comparison of the intratumoral-injected FeMSN nanoparticles. This study suggests that [email protected] composite fibres can serve as a potential localized PDT platform for effective antitumor purposes, which may spark a series of follow-on investigations for localized cancer therapeutic technology.
研究领域:
癌症治疗
·
材料科学
·
纳米技术
·
生物医学工程
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高影响因子
危险品化学品经营许可证（带存储）