JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
·
IF 9.6
Shengqin Guan,Baoen Xu,Xingbo Yu,Baixin Han,Binbin Zhang,Taotao Guan,Yu Yang,Kaixi Li,Jianlong Wang
The sluggish kinetics of oxygen evolution reaction (OER) is one of the critical challenges for electrochemical water splitting. Rational design of single atom on metal-support interactions (MSI) using deposition method is essential for electrocatalytic materials. Herein, we report the single-atomic-site and cluster-site iridium stabilized on high-entropy oxides (FeCoNiCrMoO x ) with deposition method using choline chloride/urea deep eutectic solvent (ChCl/U). The resulting Ir single atoms and clusters exhibit an average interatomic distance of approximately 0.77 nm. Ir 1&n -FeCoNiCrMoO x delivers an ultralow overpotential of 193 mV at a current density of 100 mA·cm −2 , and a long-term stability over 240 h for OER by precisely regulating the local coordination environments of the active sites in catalyst. DFT calculations reveal that closely distance single atoms and clusters exhibit stronger interactions with the high-entropy substrate. These strong interactions lead to a shift in the rate-determining step, and Ir 1&n -FeCoNiCrMoO x demonstrates the lowest theoretical OER overpotential. This work introduces DES as an effective electrochemical deposition method with synthesizing closely spaced single atoms and clusters for superior OER activity.
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AICHE JOURNAL
·
2026
·
IF 4.4
Shenhui Yu,Xingfen Huang,Xingyue Shi,Nemin Yang,Bangban Zhu,Haitao Wang,Jieyuan Zheng,Shengbin Shi,Deliang Wang,Qingyue Wang,Khak Ho Lim,Xuan Yang,Pingwei Liu,Wen-Jun Wang
Mechanistic understanding of polymerization kinetics at elevated pressure requires quantitative, time-resolved access to reaction dynamics. Herein, we developed an integrated framework coupling in situ high-pressure ATR-IR spectroscopy with a kinetic model based on the method of moments. Using ethylene/maleic anhydride (E (1)/MAH (2)) copolymerization as a benchmark, this platform enabled real-time quantification of monomer consumption and in situ determination of copolymer composition, directly confirming strict alternating incorporation. The kinetic model showed excellent agreement with experiments, with deviations below 10%. Analysis revealed the cross-propagation of MAH to ethylene-terminated radicals ( k 12 ≈ 5.62 × 10 3 L mol −1 s −1 ) is over an order of magnitude faster than the reciprocal step ( k 21 ≈ 3.92 × 10 2 L mol −1 s −1 ), identifying the latter as rate-determining. Extrapolation of the model guided the precise synthesis of a high-molecular-weight copolymer ( M w = 107 kDa). This work establishes a generalizable in situ platform for elucidating kinetics in complex polymerization systems at elevated pressure.
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ELECTROCHIMICA ACTA
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2019
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IF 5.383
Rui Lin,Lu Che,Dandan Shen,Xin Cai
How to improve durability of catalysts is the major challenge hindering the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). The alloy catalysts have been developed in efforts to reduce platinum loading, enhance catalysts activity and durability for oxygen reduction reaction (ORR) of PEMFCs. This manuscript reports the application of stepwise reduction synthesis to synthesize Pt–Ni/C and Pt–Ni–Ir/C catalysts. The synthesized electrocatalysts were characterized by X–ray diffraction (XRD), transmission electron microscopy (TEM), inductively coupled plasma mass spectrometry (ICP), X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV) and linear sweep voltammetry (LSV). The results from CV and LSV showed that when as-prepared Pt–Ni–Ir nanocrystals are uniformly dispersed on the carbon support, the catalyst exhibits excellent electrocatalytic activity and stability. When the atomic ratio of Pt, Ni, Ir is 2:2:1, after durability test of 5000 cycles, rotating disk electrode (RDE) demonstrated ORR activities of the as-prepared catalysts with the highest mass activity (MA) of 351 m A ⋅ g P t − 1 at 0.9V iR-free and electrochemically active surface area (ECSA) of 80 m 2 ⋅ g P t − 1 , which is over 17 and 2 times than those of Pt/C JM (Johnson Matthey) catalyst, respectively. This work highlights the potential to use a preparative method which means step-by-step reduction synthesis to form ternary alloy catalysts for ORR of PEMFCs.
研究领域:
电化学
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材料科学
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纳米催化
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能源材料
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燃料电池技术
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表面科学
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电催化
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiabin Ji,Congyun Zhang,Xianfeng Yang,Fanxin Kong,Chuanqiang Wu,Huimei Duan,Dongjiang Yang
Improving the sulfur-resistance of low-temperature methane combustion catalysts is great important for industrial applications. Electronic engineering of catalyst active sites is effective in tuning the catalytic performance. Herein, IrPt 0.5 /TiO 2 catalysts with electron-rich Ir structures modulated by Pt exhibit excellent low temperature sulfur-resistance towards methane combustion. The integrated characterization coupled with density functional theory calculations reveal that the strong electronic interaction between Ir and Pt induces the formation of electron-rich Ir structures. The electron-rich Ir structures with more defective oxygen vacancy and better redox ability greatly boost the adsorption and activation of O 2 while suppress SO 2 adsorption on the catalyst surface, leading to excellent sulfur tolerance towards methane combustion. This work highlights a practical electronic engineering strategy to tune the electron structure of Ir active sites for the development of practical methane oxidation catalysts.
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RENEWABLE ENERGY
·
2023
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IF 8.7
Yun Zhang,Chuanbiao Zhang,Wenjuan Li,Qiuping Xiao,Fengyuan Jiao,Sen Xu,Yanhua Lan,Yizheng Fu,Chi-Min Shu,Weiguo Cao
Stearic acid provides a basis for developing renewable energy, such as solar energy and biomass energy. A thermogravimetric-infrared spectroscopy (TG-IR) experimental test is conducted to obtain the thermal decomposition progress and the main gaseous products of stearic acid. The result shows that small gaseous products (H 2 O, CO 2 , CO, alkanes, olefins , etc.) are released. Furthermore, the method of reactive molecular dynamics simulation (ReaxFF-MD) is utilized to look into the pyrolysis reaction mechanism of stearic acid. The main pyrolysis products of stearic acid received by ReaxFF-MD are C 2 H 4 , H 2 , C 2 H 2 , CH 4 , H 2 O, CO 2 , and CO, consisting of the result of the TG-IR test. The effect of the simulated system density and temperature on the distribution of main products is also explored. Also, the thermal kinetic analysis is conducted by the initial consumption of stearic acid under different temperatures. The primary reaction mechanism of stearic acid pyrolysis is that the stearic acid molecules dissociate through C–C bonds break to generate C 2 H 4 , CH 4 , C 2 H 2 , C 3 H 6 , and other small molecules and radicals, and a typical reaction mechanism scheme of stearic acid pyrolysis is presented. The results provide a reference for explaining the macroscopic explosion characteristics of dust at the microscopic mechanism level.
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ENVIRONMENTAL TECHNOLOGY
·
2022
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IF 3.475
Zhen-xing Yang,Wen-yu Xie,Fang-fang Ye,De-hao Li
Electro-catalytic technology is a promising approach for wastewater treatment, owing to its easy operation, minimal generation of secondary pollution, small foot-print and rapid start-up. In this work, the chlorine evolution potential of the Pd-Sn modified ruthenium(Ru)-iridium(Ir) electrode was investigated for the electro-catalytic treatment of high chlorine ammonia-nitrogen wastewater. The effect of reaction conditions on the removal of ammonia-nitrogen, kinetics and apparent activation energy of ammonia-nitrogen removal were studied. The possible denitrification process of high chlorine ammonia-nitrogen wastewater was discussed. The results indicated that the chlorine evolution potential of the Pd-Sn modified Ru-Ir electrode was 1.0956 V(vs. SCE). The electro-catalytic treatment of high chlorine ammonia-nitrogen conformed to zero-order kinetic law, and the apparent activation energy of removal process was 14.089 kJ/mol. With a current was 0.5 A, the removal efficiency of ammonia-nitrogen could achieve 100% at a reaction time of 40 min. Indirect oxidation played an essential role in the electro-catalytic ammonia-nitrogen removal using the Pd-Sn modified Ru-Ir electrode. This paper demonstrated that the electro-catalytic technology was a promising approach for efficiently treating the high chlorine ammonia-nitrogen wastewater.
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ChemistrySelect
·
2022
·Vol. 7
·期 31
·e202201268
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IF 2.307
Aixiao Fu,Mengqing Sun,Shifeng Jiang,Huanfei Xu,Guoqiang Xu
Graphical Pyrroles are important nitrogen-containing compound. Here, we constructed N, P-doped activated carbon supported Ir to perform the synthesis of pyrroles from alcohols and amino alcohols. The unique performance is attributed to the interaction between Ir and N, P-doped activated carbon. Pyrroles are a significant class of nitrogen-containing heterocyclic compounds and the derivatives. Here, an efficient procedure has been proposed for the loading of Ir on N, P-doped activated carbon to exploit pyrroles are synthesized from alcohols and amino alcohols. And the optimal conversion of 1-phenylethanol is up to 65 % with 2-phenylpyrrole selectivity of 80 %. The good performance is attributed to the interaction between metal Ir and N, P-doped activated carbon, which could also be confirmed from BET and XPS characterizations. What's more, the catalyst could be generally used for a range of reactions to produce pyrroles from alcohols and amino alcohols.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 22
·8832-8839
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IF 4.569
Yihao Gao,Jie Bai,Tianning Zhou,Yaqiong Gong
In recent years, Co-based metal–organic frameworks (Co-MOFs) have received significant research interest because of their large specific surface area, high porosity, tunable structure and topological flexibility. However, their comparatively weak electrical conductivity and inferior stability drastically restrict the application of Co-MOFs in the synthesis of electrocatalysts. In this study, ZIF-67 was grown on nickel foam by a room temperature soaking method, and then Ir–Co(OH)2@ZIF-67/NF was assembled by a hydrothermal method. The prepared Ir–Co(OH)2@ZIF-67/NF nanosheets exhibit remarkable conductivity, larger electrochemical active surface area and wider electron transport channels. Only ultralow overpotentials of 198 mV, 263 mV, and 300 mV were needed for Ir–Co(OH)2@ZIF-67/NF to reach the current densities of 10 mA cm−2, 50 mA cm−2, 100 mA cm−2, meanwhile, no obvious degradation of the current density at 10 mA cm−2 was observed for about 16 h. This work may provide a promising strategy for developing high-performance MOF-derived materials as electrocatalysts for the OER under alkaline conditions.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 28
·期 3
·e202103346
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IF 5.236
Zhongxian Fan,Jiaen Xie,Tumpa Sadhukhan,Chao Liang,Can Huang,Wenqing Li,Tingxuan Li,Pingyu Zhang,Samya Banerjee,Krishnan Raghavachari,Huaiyi Huang
Graphical Four novel Ir(III) photo-catalysts ( Ir1 – Ir4 ) were synthesized and applied for photocatalytic cancer therapy. Upon blue and green light irradiation, these photocatalysts generated singlet oxygen and induced rapid photo-catalytic oxidation of the cellular coenzymes NAD(P)H. Ir2 triggered promising photo-induced anticancer activity via induction of intracellular redox imbalance and exhibited ideal in vivo photo-induced catalytic anticancer activity. Four photo-catalysts of the general formula [Ir(CO6/ppy) 2 (L)]Cl where CO6=coumarin 6 ( Ir1 – Ir3 ), ppy=2-phenylpyridine ( Ir4 ), L=4′-(3,5-di-tert-butylphenyl)-2,2′ : 6′,2′′-terpyridine ( Ir1 ), 4′-(3,5-bis(trifluoromethyl)phenyl)-2,2′ : 6′,2′′-terpyridine ( Ir2 and Ir4 ), and 4-([2,2′ : 6′,2′′-terpyridin]-4′-yl)-N,N-dimethylaniline ( Ir3 ) were synthesized and characterized. These photostable photo-catalysts ( Ir1 – Ir3 ) showed strong visible light absorption between 400–550 nm. Upon light irradiation (465 and 525 nm), Ir1 – Ir3 generated singlet oxygen and induced rapidly photo-catalytic oxidation of cellular coenzymes NAD(P)H. Ir1 – Ir3 showed time-dependent cellular uptake with excellent intracellular retention efficiency. Upon green light irradiation (525 nm), Ir2 provided a much higher photo-index (PI=793) than the clinically used photosensitizer, 5-aminolevulinicacid (5-ALA, PI>30) against HeLa cancer cells. The observed necro-apoptotic anticancer activity of Ir2 was due to the Ir2 triggered photo-induced intracellular redox imbalance (by NAD(P)H oxidation and ROS generation) and change in the mitochondrial membrane potential. Remarkably, Ir2 showed in vivo photo-induced catalytic anticancer activity in mouse models.
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LANGMUIR
·
2021
·
IF 3.882
Hongbo Yu,Jihao Zhao,Chunzheng Wu,Bo Yan,Shuangliang Zhao,Hongfeng Yin,Shenghu Zhou
Decoration of noble metals with transition-metal oxides has been intensively studied for heterogeneous catalysis. However, controllable syntheses of metal–metal oxide heterostructures are difficult, and elucidation of such interfaces is still challenging. In this work, supported IrCo alloy nanoparticles are transformed into supported Ir–CoOx close-contact nanostructures by in situ calcination and following selective reduction. Relative to Ir/Al2O3, Ir–CoOx/Al2O3 shows greatly enhanced activities for the hydrogenation of furfural derivatives to the corresponding furfuryl alcohol derivatives with more than 99% selectivity and demonstrates significantly improved activities and selectivity for hydrogenations of α,β-unsaturated aldehydes to α,β-unsaturated alcohols. The modification of Ir surfaces with CoOx prevents Ir nanoparticles from growing, achieving high thermal and catalytic stabilities. Theoretic calculation suggests that the better catalytic performance of Ir–CoOx/Al2O3 is ascribed to the Ir–CoOx interaction, which promotes the absorption of furfural as well as desorption of furfuryl alcohol, resulting in enhanced catalytic activities.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuhua Xie,Xinxin Yu,Xianwei Li,Xue Long,Chaofeng Chang,Zehui Yang
The industrialization of solid polymer electrolyte water electrolysis (SPEWE) dominantly relies on electrocatalyst with high stability and efficiency for oxygen evolution reaction (OER) catalysis. In this work, we report a facile method to construct α-Ni(OH) 2 @Ir core–shell nanoparticles as bifunctional electrocatalyst for acidic overall water splitting application. α-Ni(OH) 2 @Ir requires lower overpotentials (238 mV and 20 mV) to achieve 10 mA cm −2 in acidic OER and HER catalysis compared to benchmarked IrO 2 (332 mV) and Pt/C (36 mV); meanwhile, the OER mass activity at 1.55 V vs. RHE was 92 fold higher than IrO 2 ; HER mass activity at overpotential of 80 mV was 5 fold better than Pt/C. The boosted catalytic activity is due to the enhanced utilization efficiency of Ir stemmed from the ultrathin Ir shell (~1 nm). Moreover, 1.49 V is demanded for α-Ni(OH) 2 @Ir to attain 10 mA cm −2 in acidic overall water splitting, 110 mV lower than benchmarked Pt/C-IrO 2 system. Meanwhile, stable catalytic performance is recorded for 20 h.
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Journal of Biophotonics
·
2021
·Vol. 14
·期 11
·e202100117
·
IF 3.207
Lijun Zhu,Jianjun Chen,Ting Yan,Gulinigaer Alimu,Xueliang Zhang,Shuang Chen,Mutalifu Aimaiti,Rong Ma,Nuernisha Alifu
Photothermal therapy (PTT) has attracted wide attention due to its noninvasiveness and its thermal ablation ability. As photothermal agents are crucial factor in PTT, those with the characteristics of biocompatibility, non-toxicity and high photothermal stability have attracted great interest. In this work, new indocyanine green (IR-820) was utilized as a photothermal agent and near-infrared (NIR) fluorescence imaging nanoprobe. To improve the biocompatibility, poly(styrene-co-maleic anhydride) (PSMA) was utilized to encapsulate the IR-820 molecules to form novel IR-820@PSMA nanoparticles (NPs). Then, the optical and thermal properties of IR-820@PSMA NPs were studied in detail. The IR-820@PSMA NPs showed excellent photothermal stability and biocompatibility. The cellular uptaking ability of the IR-820@PSMA NPs was further confirmed in HeLa cells by the NIR fluorescent confocal microscopic imaging technique. The IR-820@PSMA NPs assisted PTT of living HeLa cells was conducted under 793 nm laser excitation, and a high PTT efficiency of 73.3% was obtained.
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