Plasma Processes and Polymers
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2017
·Vol. 15
·期 4
·1700176
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IF 2.846
Lei Wang,Jinxiu Wang,Junxin Lin,Songlin Zhang,Yongjun Liu
Degradation of metronidazole (MNZ) by radio frequency discharge in water was examined. Results showed that • OH, H • , and • O were produced. Decay of MNZ followed pseudo-first order kinetics, where the apparent rate constant was independent of its initial concentration in the range 0–0.5 mM, decreased in the range 0.5–1.0 mM, and leveled off in the range higher than 1.0 mM. pH had no effects on MNZ degradation. • OH scavengers enhanced the MNZ removal. Formic acid, nitrite ion, oxalic acid, nitrate ion, and acetic acid were determined as the primary intermediate byproducts. The eventual products were ammonia and inorganic carbon. Both • OH and H • participated in the MNZ degradation. H • played more efficient role than • OH in the early stage.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
Journal of the American Chemical Society
·
2020
·
IF 14.612
Jie Li,Guangming Zhan,Jianhua Yang,Fengjiao Quan,Chengliang Mao,Yang Liu,Bo Wang,Fengcai Lei,Lejing Li,Alice W. M. Chan,Liangpang Xu,Yanbiao Shi,Yi Du,Weichang Hao,Po Keung Wong,Jianfang Wang,Shi-Xue Dou,Lizhi Zhang,Jimmy C. Yu
The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat–1 h–1), a small partial current density (<1 mA cm–2), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat–1 h–1) than the Haber–Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen–hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm–2 current densities for 100 h due to the robust subsurface Ru–O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis.
研究领域:
化学工程
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电催化
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材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Xiaoye Geng,Wei Gao,Haipeng Jiang,Guoliang Li,Fengyu Zhao,Weichen Wang
Aluminum (Al) is an attractive material for hydrogen generation through its reaction with water. This study assesses the effectiveness of aluminum hypophosphite (AHP) in inhibiting Al dust explosions and elucidates its decomposition pathway and inhibition mechanism. At a concentration of 1050 g/m 3 , AHP completely inhibited the maximum explosion intensity of Al dust. Its high activation energy and P–O cross-linking layer impeded heat transfer. Reactive force field molecular dynamics (ReaxFF-MD) simulations complemented that AHP decomposes into vital products such as PH 2 and H 2 PO 2 . Concurrently, CHEMKIN numerical calculations highlighted the crucial role of phosphorus hydroxide (PH) radicals in the recycling and regeneration of phosphorus radicals. The reaction PO 2 + PH⇔ HOPO + P accelerated the cycling of HOPO, thereby reducing the required radicals for sustaining aluminum combustion. AHP exhibits dual-phase inhibition against Al dust explosions, thereby guaranteeing the safe operation of aluminum-based hydrogen generation systems in the hydrogen energy domain.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Jun Zhang,Shuyue Liu,Shiyu Lu,Chunyuan Wang,Pingjuan Liang,Huan Yi,Mengjie Li,Laizheng Luo,Rong Wang,Guangming Jiang
Improving the utilization of hydrogen radicals (H*) is of great significance for effective Pd-mediated electrocatalytic hydrodechlorination (EHDC) in detoxifying chlorinated organic pollutants (COPs). However, the limited H* utilization by single Pd arises from its inadequate performance in adsorbing/activating COPs and inferior mass transfer of low-concentration COPs. In this study, an urchin-like yolk/shell TiO 2 spheres with mesoporous structure are developed for supporting Pd nanoparticles (Pd/U-TiO 2 ), which exhibits superior EHDC activity and selectivity for 2,4-DCP reduction. Notably, the prepared Pd/U-TiO 2 catalyst achieves a mass activity of 4.2 min −1 g Pd -1 and a specific activity of 1.94 min −1 mol Pd -1 when detoxifying 50 mg/L of 2,4-DCP at −0.85 V, surpassing the most reported catalysts. Furthermore, the Pd/U-TiO 2 catalyst consistently demonstrates higher H* utilization efficiency compared to single Pd, regardless of the 2,4-DCP concentration or reaction mode (batch or continuous-flow). This enhanced H* utilization efficiency is attributed to two key factors: the urchin-like and yolk/shell structure of U-TiO 2 enhances the mass diffusion of 2,4-DCP, and the strong interactions between Pd and U-TiO 2 generate electron-rich Pd species that enhance the adsorption and activation of COPs. Overall, this work highlights the synergistic effects of strong metal-support interactions and mass diffusion in enhancing atomic H* utilization. This study lays a significant experimental and theoretical foundation for designing efficient electrocatalysts for the detoxification of chlorinated organic pollutants and various other halogenated organic pollutants.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Yao Zhibo,Cheng Hao,Xu Yifei,Zhan Xinyu,Hong Song,Tan Xinyi,Wu Tai-Sing,Xiong Pei,Soo Yun-Liang,Li Molly Meng-Jung,Hao Leiduan,Xu Liang,Robertson Alex W.,Xu Bingjun,Yang Ming,Sun Zhenyu
The electrocatalytic reduction of CO 2 to CO is slowed by the energy cost of the hydrogenation step that yields adsorbed *COOH intermediate. Here, we report a hydrogen radical (H•)-transfer mechanism that aids this hydrogenation step, enabled by constructing Ni-partnered hetero-diatomic pairs, and thereby greatly enhancing CO 2 -to-CO conversion kinetics. The partner metal to the Ni (denoted as M) catalyzes the Volmer step of the water/proton reduction to generate adsorbed *H, turning to H•, which reduces CO 2 to carboxyl radicals (•COOH). The Ni partner then subsequently adsorbs the •COOH in an exothermic reaction, negating the usual high energy-penalty for the electrochemical hydrogenation of CO 2 . Tuning the H adsorption strength of the M site (with Cd, Pt, or Pd) allows for the optimization of H• formation, culminating in a markedly improved CO 2 reduction rate toward CO production, offering 97.1% faradaic efficiency (FE) in aqueous electrolyte and up to 100.0% FE in an ionic liquid solution.
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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产品关联
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2025
·
IF 6
Fengjiao Quan,Pengfei Xu,Xiufan Liu,Wenjuan Shen,Yuhao Li,Jianfen Li,Yun He,Fangyuan Chen
Nitrate (NO 3 − ) pollution in groundwater has emerged as a pressing environmental issue of global concern. The excessive application of chemical fertilizers is widely recognized as the primary contributor to this pollution Nitrate ions pose significant risks to human health and the ecological environment. Electrochemical reduction of NO 3 − to NH 3 (NITRR) represents an effective approach for nitrogen recovery and recycling. Among many electrode materials, copper-based catalysts were considered promising due to their low cost and strong NO 3 − conversion capability. However, excessively strong adsorption can lead to catalyst deactivation, thereby diminishing catalytic activity. In this study, we developed an electrode material (Cu@NiO/NF) with low-valent copper (Cu δ+ ) through the combination of Cu and NiO, and it exhibited excellent catalytic performance in the NITRR process. At − 0.45 V vs. RHE, this catalyst achieved a Faraday efficiency of 95.7 % and an ammonia yield of 0.85 mg h −1 cm −2 . Further experiments and theoretical calculations demonstrate that the presence of NiO in Cu@NiO/NF stabilizes Cu δ+ , thereby enhancing the charge transfer rate and promoting the formation of hydrogen radicals (H•). This work has pioneered a new avenue for the development of efficient and innovative NTIRR materials.
研究领域:
环境科学
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电化学
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催化
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材料科学
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水污染控制
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产品关联
DOI
高影响因子
ChemCatChem
·
2025
·
IF 3.9
Hengyu Zhao,Jing Zhao,Xue Li,Bate Nasen,Yang Wu,Xinlong Wang,Jinxiong Wu,Yaya Wang
The catalytic reduction of 4-nitrophenol (4-NP), a persistent environmental pollutant faces dual challenges reliance on noble metals and inefficient utilization of hydrogen radicals (H*). Meanwhile, nickel-containing sludge generated by the electroplating industry, classified as hazardous waste has long posed significant disposal conundrums. Herein, we developed a noble metal-free pyroxene-type CaNi(Si 2 O 6 ) catalyst, synthesized from electroplating sludge, that simultaneously addresses these challenges through dynamically reconstructed Ni–O–Ca interface with oxygen vacancies and interfacial electron transfer channels. Ni@Ca-195/20 establishes a self-sustaining catalytic system, achieving a remarkable conversion of 96.8% with 0.1 mM NaBH 4 and 0.05 mg catalyst, while maintaining stability over 31 cycles in low concentration regimes. Integrated characterization combined with catalytic performance evaluation reveals an interfacial electron transfer mechanism: the engineered interface enables in situ reduction of Ni 2+ generates metallic electron-deficient Ni δ+ species, enhancing 4-NP − and BH 4 − adsorption through dual-site coordination. Oxygen vacancies accelerate BH 4 − hydrolysis, while electron transfer channels sustain H* flux via Ca 2+ modulated charge equilibration. This work establishes a waste-to-functionality paradigm for designing defect-engineered catalysts while advancing sustainable remediation of nitroaromatic pollutants. Graphical The Ni-plating sludge was converted into a Ni@Ca-195/20 catalyst with abundant oxygen vacancies and Ni–O–Ca heterointerfaces via the solvothermal method, which was used to efficiently catalyze the hydrogenation reduction of 4-nitrophenol.
研究领域:
环境催化
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废物资源化
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材料化学
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污染治理
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shiyu Zuo,Yan Wang,Jinquan Wan,Chao Yang,Lulu Wang,Pengfei Ou
Hydrodefluorination is a selective and gentle approach for the safe treatment of fluorinated pollutants; however, the efficient production of hydrogen-radical (H·) active species remains a major challenge, particularly under alkaline conditions. Herein, we synthesized two iron- and nitrogen-co-doped carbon (FeNC) catalysts, FeNC-pyridine N and FeNC-pyrrole N, which have different N coordination structures. Through theoretical prediction and experimental verification, we elucidated the regulatory and improving effects of the electronic structure, through N configuration, to enhance H· generation. Particularly, FeNC-pyridine N exhibited increased electron localization, a higher electron density, a lower work function, and stronger proton affinity, which significantly enhanced H + adsorption and its subsequent reduction to H·, thereby accelerating the hydrodefluorination process. This reaction not only facilitates pollutant oxidation but also prevents the formation of highly toxic, short-chain fluorinated byproducts. We reveal the critical role of N coordination in FeNC catalysts in promoting hydrodefluorination and the oxidative removal of fluorinated pollutants, offering new insights into the safe remediation of these pollutants.
研究领域:
环境化学
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催化
·
材料科学
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污染物修复
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
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