GREEN CHEMISTRY
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2025
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IF 9.2
Xueqi Liu,Jingmin Ge,Shiying Li,Huanhuan Yang,Huiwen Tian,Hongpo Liu,Yaxi Li,Xiaoli Zheng,Yapeng Tian,Xinwei Cui,Qun Xu
Identification of the active sites for zinc oxide-derived catalysts and further elucidation of the catalytic mechanism for electrochemical CO2 reduction reaction (CO2RR) are limited by the dynamic structural evolution at real reaction conditions. Herein, we focus on the structural evolution of ZnO-T at the initial stage of CO2RR. ZnO-T undergoes in situ reduction to Zn within dozens of minutes, which is followed by reoxidation of the out layer. As a result, core-shell-like Zn@ZnO-T with controllable Zn-ZnO interfaces and oxygen vacancies is obtained depending on the temperature-controlled annealing and electrochemical pre-treatment. Zn-ZnO interfaces alter the energy band structure of ZnO layer, while oxygen vacancies modify the electron density of Zn sites. Thus, the obtained Zn@ZnO-T improves charge transfer, facilitates CO2 activation, and lowers energy barrier for *COOH and *CO intermediates formation. Expectedly, Zn@ZnO-T demonstrates excellent CO2RR performance for CO production with FE up to 92.1% at −1.2 V (vs. RHE) and a current density of −12.7 mA∙cm−2. In particular, Zn@ZnO-650 delivers a high FECO above 85% over a wide potential range from −1.0 to −1.3V (vs. RHE). This study provides a new compass for mechanistic investigation on relationship between intrinsic structure and catalytic performances, guiding the rational design of high-performance heterogeneous catalysts.
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DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 37
·19159-19164
·
IF 6.895
Songliang Liu,Ziqiang Wang,Hugang Zhang,Shuli Yin,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Adjusting the morphology and composition of Pd-based materials is a promising strategy to improve their performance for the electrocatalytic formic acid oxidation reaction (FAOR). In this work, we report the preparation of B-doped PdRu nanopillar assemblies (B-PdRu NPAs) by a two-step method using NaBH4 as the boron dopant. On combining the hyper-branched structure and the multi-component synergistic effect, B-PdRu NPAs achieve a high mass activity of 1.09 mA μg−1Pd for the FAOR and retain 73.19% of the initial activity after 500 cycles, which is superior to undoped counterparts. The proposed synthesis strategy provides a simple method for the synthesis of metal–nonmetal nanomaterials with desired composition and design structure for electrocatalytic fields.
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PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2018
·
IF 3.716
Qing Liu,Kevin Yan,Qiaomei Chen,Soumia Cheddah,Lin Shen,Han Xiao,Yan Wang,Chao Yan
Capillary column packed with silica colloidal crystals (SCC) exhibits great efficiency in liquid chromatography because of its highly-ordered structure and extremely narrow channels (about hundred nanometer in diameter) between the particles. However, problems arise due to the extremely high back-pressure created with its dense packings. It is also a challenge to prepare a stable SCC column with an appropriate length for chromatographic separation on a commercial instrument. We have synthesized monodispersed, sub-micron SiO 2 particles bonded with C18 functionality and fabricated SCC capillary columns up to 100 mm in length. The packing materials in the column displayed Bragg diffraction with blueish color under irradiation with white light, indicating the formation of SCC. The column performance was evaluated using pressurized capillary electrochromatography (pCEC) and column efficiencies of more than a hundred thousand plates per column (plate height < 1 μm) were achieved using peptide as a sample. The run-to-run reproducibility expressed with RSD in terms of retention time and peak area for aromatic compounds were less than 0.076% and 1.96%, respectively. These results demonstrate that the combination of pCEC and SCC columns may provide an innovative analytical technique with extraordinary efficiency, resolution and speed for the separation of complex samples.
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高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Daoqing Fan,Shuai Qin,Chuanping Li,Yujia Ren,Lilin Hao,Hengqian Zhang,Jiawen Han,Jingyu Hou,Juan Wang,Shaojun Dong
Rational design of high-performance nanozymes with multiple enzyme-mimicking activities for biochemical sensing is one of the most promising directions in this area. D-PA is a kind of S-containing pharmaceutical for treating various diseases; the side effects caused by its unreasonable intake/residual have posed severe threats to human health and the living environment, making its accurate analysis gradually significant. However, most previous works exhibited the drawbacks of complicated synthesis of nanomaterials, unreliable single-modal results, and limited portable sensing ability. Herein, we prepared a low-cost MoCu-2MI MOF nanozyme via a simple hydrothermal method and revealed its excellent peroxidase/laccase dual-enzyme-mimicking properties that might benefit from a bimetallic valence modulation strategy via multifaceted experiments (EIS, EPR, ROS probes, and Michaelis-kinetic tests). Initially, MoCu-2MI MOF worked as a POD mimic and catalyzed the oxidation of TMB into blue-colored Ox-TMB. By synergistically harnessing the visual/photothermal effect of Ox-TMB and the effective reduction and ROS-scavenging abilities of D-PA, we constructed the first colorimetric-RGB-photothermal trimodal D-PA sensor with the assistance of portable devices, bringing evidently strengthened cost-effectiveness, reliability, and portable sensing ability. The LODs for D-PA under the three modes were 0.24, 7.88, and 7.98 μM, which could compete with most previous works. Moreover, the trimodal sensor presented satisfactory applicability in human serum and milk samples. More surprisingly, taking 2,4-DP as the model target (LOD = 0.11 μM), we further achieved the visual analysis of phenolic pollutants based on the excellent LAC-like activity of MoCu-2MI MOF. This work not only offered an effective approach for the exploration and controllable modulation of nanozymes with multiple enzyme-like properties but also opened up unique horizons for the design of multimodal portable biosensors.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Peiwen Wu,Kailong Yu,Shuaishuai Zhou,Jing He,Haiyan Ji,Linlin Chen,Yan Huang,Hui Liu,Jixing Liu,Huaming Li,Wenshuai Zhu
Efficient oxidative desulfurization (ODS) of aromatic sulfur compounds under mild and green conditions remains a major challenge due to the limited activation ability of molecular oxygen and poor stability of traditional catalysts. In this work, a series of HPMo@MIL-100 catalysts were synthesized for ODS of fuel oils using molecular oxygen as a green oxidant. The introduction of HPMo into the MIL-100 framework not only improved the catalytic performance but also significantly regulated the electronic environment of the Fe active centers. Structural and electronic characterizations confirmed that HPMo incorporation decreased crystallinity, increased surface defects, and facilitated electron transfer within the framework. Detailed experiments identified superoxide radicals as the dominant reactive species, efficiently generated under the synergistic effect of HPMo and MIL-100. The optimized catalyst, HPMo@MIL-100–2, achieved complete removal of aromatic sulfides within 3 h at 120 °C and the aromatic sulfides were selectively conversed to corresponding sulfones. In addition, the catalyst demonstrated excellent recyclability, which can be reused 9 times without significant decrease in ODS performance. Furthermore, a desulfurization efficiency of 95.7 % was achieved to real FCC diesel, highlighting the catalyst’s potential for industrial application. This study provides an effective strategy for tuning MOF catalytic systems through electron modulation, enabling highly efficient, selective, and recyclable ODS performance under mild conditions.
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高影响因子
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