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ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY · 2016 ·Vol. 22 ·期 3 ·327-334 · IF 1.87

Perovskite LaMnO3/ZSM-5 composites for H2S reactive adsorption at high temperature

Liu Dongjing,Zhou Weiguo,Wu Jiang

Perovskite LaMnO 3 /ZSM-5 was used for reactive adsorption of hydrogen sulfide at 500–700 °C. The sorbents showed good desulphurization performance, the highest sulfur capacity of 1020 µmol S/g over 5La5Mn/ZSM-5 was obtained at 600 °C. The reducing gases (H 2 and CO) can obviously shorten the breakthrough time and reduce the sulfur capacity. Incorporating Mn ions into La 2 O 3 lattice improved the sulfidation activity due to the formation of perovskite LaMnO 3 with good reducibility and structure stability.

CAS / MDL: 10277-43-7 20694-39-7
研究领域: 材料科学 · 环境工程
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MATERIALS LETTERS · 2019 · IF 3.019

Tuning the electron status of urchin-like CoS2 nanowires by selenium doping toward highly efficient hydrogen evolution reaction

Yuqiao Wang,Chuanyong Jian,Wenting Hong,Qian Cai,Wei Liu

Cobalt disulfide (CoS 2 ) for hydrogen evolution reaction (HER) suffers from unfavorable hydrogen adsorption properties due to the strong interaction between the adsorbed H and the intensely electropositive cobalt atom. Herein, we successfully demonstrate a general strategy to improve the hydrogen evolution activity of CoS 2 by modulating the surface electron density. The selenium doped CoS 2 (Se-CoS 2 ) nanowires arrays exhibit a durable activity for electrochemical hydrogen evolution in 0.5 M H 2 SO 4 solution to deliver 10 mA cm −2 at the overpotential of only 139 mV. Our density functional theory studies consistently confirm that the surface electron density of CoS 2 has been effectively manipulated by Se doping. The adsorbed hydrogen binding energy to Se-CoS 2 can be optimized to provide an optimal condition for electron and proton transferring to the adsorbed H 2 , thereby promoting HER activity of CoS 2 .

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

In-plane carrier regulation and hydrogen adsorption/desorption optimization of P4 molecule anchored Vs-ZnIn2S4−x for improve photocatalytic activity

Qingjie Luan,Xiangdong Xue,Hongtai Feng,Lu Tao,Dongxue Zhou,Tengfei Chen,Mengxi Tan,Wenjun Dong

Molecular-type cocatalysts can achieve the maximum electron transfer and minimum light absorption loss by virtue of their size advantage. Herein, a novel hydrophilic molecule-semiconductor hybrid P 4 @Vs-ZnIn 2 S 4−x photocatalyst was successfully developed by in-situ P 4 molecular anchoring on S defect ZnIn 2 S 4−x (V S -ZnIn 2 S 4−x ). The electron-rich P 4 molecules are anchored on the Zn-S 4 surface through S vacancies, forming Zn-P and S-P bonds that can promote electron injection from the electron-rich P 4 molecular to Vs-ZnIn 2 S 4−x substrate and reduce the adsorption/desorption barrier of H intermediate on S atom of Zn-S 4 plane. Meanwhile, the electrostatic potential depression around P 4 promoted the directional migration of in-plane photogenerated electrons, and pooled electrons to the highly active P sites and S sites, thereby accelerating the kinetics of hydrogen evolution. As a result, P 4 @Vs-ZnIn 2 S 4−x achieves an optimal photocatalytic hydrogen evolution activity of 26.1 mmol g −1 h −1 under visible light, which is 6.2 times higher than 4.2 mmol g −1 h −1 for Vs-ZnIn 2 S 4−x .

研究领域: 材料科学 · 化学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Tuning the amphiphilicity of terpyridine-based fluorescent probe in water: Assembly and disassembly-controlled H g2+ sensing, removal, and adsorption of H2S

Guilin Zhou,Xiaodong Zhang,Xin-Long Ni

A water-soluble terpyridine-based cationic fluorescent probe ( SP - TPy ) was synthesized, which emerged with pH-dependent amphiphilicity, resulting in self-assembly and disassembly in aqueous media with the aggregation-induced emission (AIE) property. In neutral water (pH 7.4), a moderate sensing response to Hg 2+ ions was given by the self-assembly of SP - TPy . However, in acidic aqueous media, the monomer of SP - TPy not only appeared to be highly selective and sensitive for Hg 2+ ions, but also displayed highly efficient removal of Hg 2+ ions from solution by rapid precipitation, which was attributed to the coordination-triggered reassembly of SP - TPy . The removal efficiency of SP-TPy f or Hg 2+ was found to be over 99%. Further study indicated that the precipitates were composed of various polyhedral porous frameworks, a property that was further used to adsorb H 2 S gas to form HgS complexes with higher uptake capacities. In addition, SP - TPy can be efficiently regenerated and recycled using a simple treatment with acidic water after adsorption of the H 2 S gas.

研究领域: 化学 · 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Regulation of water and sulfur resistance and study of carbon dioxide adsorption properties on FAU zeolites

Yifan Zhang,Yangyang Guo,Shanshan He,Honglin Guo,Lei Luo,Mengran Li,Tingyu Zhu,Tao Guo,Yanxi Deng

CO 2 capture from blast furnace gas is of great significance for carbon reduction. 13X zeolites are frequently employed as CO 2 adsorbents. Nevertheless, their large-scale utilisation in industrial applications is impeded by the presence of H 2 O and H 2 S in blast furnace gas. To develop CO 2 adsorbents suitable for carbon capture from blast furnace gas, a series of Faujasite (FAU) zeolites were prepared in this study by modulating Si/Al. The findings revealed that the separation coefficients of CO 2 /N 2 and CO 2 /CO increased by 72 % and 144 %, respectively, and that the H 2 O adsorption decreased by 23 % when Si/Al was increased from 1.45 to 2.93. Furthermore, breakthrough experiments demonstrated that enhancing the Si/Al ratio of FAU zeolite can effectively reduce the dynamic adsorption capacity of H 2 O and H 2 S. Physicochemical characterizations of the zeolite before and after H 2 S adsorption were performed: CO 2 and N 2 adsorption isotherms, thermogravimetry, In-situ FT-IR and XPS. The present study investigates the effect of H 2 S adsorption on zeolites with varying Si/Al ratios. When combined with DFT calculations, the results demonstrate that the elevated Si/Al ratio of the zeolite results in a significant increase in sulfur resistance and easier deposition of H 2 S in the form of sulfate on the zeolite surface. It indicates that the modulation of Si/Al ratio is an effective method to improve the water and sulfur resistance of zeolites, and provides core material support for the practical application of large-scale carbon capture technology for blast furnace gas.

CAS / MDL: 11138-49-1 112926-00-8
研究领域: 材料科学 · 环境科学 · 化学工程
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CARBON · 2015 · IF 6.196

Molten salt synthesis of nitrogen-doped porous carbons for hydrogen sulfide adsorptive removal

Zhengfa Yu,Xuzhen Wang,Xuedan Song,Yang Liu,Jieshan Qiu

Nitrogen-doped porous carbons (NPCs) with high hydrogen sulfide (H 2 S) adsorption capacity have been prepared through the molten-salt approach, using d -glucose as carbon source, melamine as nitrogen source and eutectic salt (LiCl/KCl) as porogen. The NPCs possess tunable nitrogen content (3.07–24.31 wt.%) and specific surface area (451–1190 m 2 /g) with the changing of the weight ratio of nitrogen source to carbon source and synthesis temperature. The H 2 S adsorptive performance of NPCs is highly superior to that of non-doped porous carbon . X-rays photoelectron spectroscopy analyses combined with quantum chemical calculations demonstrate that the adsorption performance of the as-prepared NPCs depends on their nitrogen content and N-bonding configurations in the carbon materials, as well as their porosity. Pyridinic nitrogen doped carbon in NPCs have stronger interaction with H 2 S compared to pyrrolic and graphitic nitrogen doped carbon. Based on the advantages of the developed porosity and abundant nitrogen functional groups, the saturated sorption capacities of 0.97–1.25 mmol H 2 S/g can be achieved over NPCs at 25 °C under dry and anaerobic conditions .

CAS / MDL: 7447-41-8
研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Better than Pt in all-pH media: A charge transfer modulating hydrogen adsorption in cobalt-rhodium alloy aerogel to boost hydrogen evolution

Su Yan,Xia Yang,Mengxiao Zhong,Weimo Li,Xiaojie Chen,Jiaqi Xu,Wei Chen,GuangTao Yu,Ce Wang,Xiaofeng Lu

In this study, a series of X-Rh (X = Fe, Co, Ni) alloy aerogels (AGs) are constructed via a galvanic replacement strategy. Due to the optimized electronic structure and the unique features of metal aerogel, the resultant Co AG-Rh500 electrocatalyst exhibits much better HER activity and robust stability than the benchmark commercial Pt/C catalyst in all-pH media. Theoretical result further reveals that the top sites of Co and Rh atoms in the (0   0   1) and (1   0   0) surfaces of the hybrid CoRh alloy systems can act as the active sites especially in an acidic condition, while the bridge and hollow sites on the (0   0   1) and (1   0   0) surfaces of CoRh alloy contribute a lot to the superior HER kinetics in alkaline and neutral electrolytes. Furthermore, the apparent electron transfer between Co and Rh atoms modulates the adsorption state of H*, thereby promoting the HER performance.

CAS / MDL: 15336-18-2
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Boosting hydrogen adsorption via manipulating interfacial electronic structure of NiPx for enhanced alkaline seawater electrolysis

Xu Chen,Yunrui Duan,Huanglin Dou,Wensheng Zhang,Xiaomin Wang

The development of transition metal phosphides (TMPs) electrocatalysts with appropriate binding strength towards intermediates and resistant to chlorine in alkaline seawater electrocatalysis remains a formidable challenge. Herein, an approach for manipulating electron redistribution in Ni 2 P/Ni 5 P 4 treated by Co cationic doping engineering (denoted as Act-Co-NiPx) is proposed, exhibiting excellent catalytic activities and stability toward HER in alkaline seawater solution. First-principles calculations demonstrate that the Co doping can effectively adjust the electron redistribution of Ni 2 P/Ni 5 P 4 , resulting in a reduction in the hydrogen adsorption free energy for HER and an acceleration in the interfacial charge transfer. Furthermore, the enhanced Cl - adsorption energy avoids the toxicity of Cl - to the active sites in alkaline seawater splitting. Consequently, the resulting Act-Co-NiPx catalyst demonstrates remarkable HER performance with low overpotentials of 77 and 97 mV at a current density of 10 mA cm −2 in both 1.0 M KOH and 1.0 M KOH+Seasalt electrolytes. Furthermore, the seasalt electrolyzer assembled from Act-Co-NiPx achieves the low cell voltage of 1.63 V at 10 mA cm −2 . This work demonstrates a feasible method for designing cost-effective and stable catalysts with excellent selectivity via regulating the electronic structure of TMPs for seawater electrolysis.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Overcoming Interfacial Hydrogen Site-Blocking during Alkaline Formate Oxidation: Insights from Lattice-Compressed PdZr/C Catalysts

Lanlan Shi,Feike Zhang,Xiaojun Wang,Jingxian Li,Yuanming Liu,Weijie Fu,Shuyun Yao,Shiyu Wang,Kang Ji,Yingjie Ji,Zhiyu Yang,Jiangzhou Xie,Yi-Ming Yan

Improving the electrocatalytic conversion of formate in alkaline solutions is crucial for the commercial application of formate fuel cells. However, palladium-based catalysts used for formate oxidation reactions (FOR) face challenges due to the strong adsorption of hydrogen intermediates, resulting in lower catalytic efficiency in alkaline environments. Herein, we prepared a PdZr/C catalyst aimed at employing a doping-induced strain strategy to reduce the hydrogen binding energy of palladium and release more active sites for the oxidation of formate. Through density functional theory calculations and experimental investigations, we find that the lattice compression induced by Zr doping regulates the electronic structure of Pd. Specifically, the incorporation of Zr dopant shifts the d-band center of Pd downward, weakening the binding energy of hydrogen at the Pd sites. This adjustment promotes the desorption of hydrogen intermediates, thus accelerating the FOR kinetics by alleviating the site-blocking effect. As a result, the PdZr/C catalyst exhibited a 2.4-fold increase in activity compared to the conventional Pd/C catalyst. It also achieved a lower peak potential and delivered a significantly higher peak current of 1917 mA mg–1. These findings highlight the critical role of lattice strain in tuning the catalytic properties of Pd and offer valuable insights into the design of high-performance electrocatalysts for energy conversion technologies.

研究领域: 材料科学 · 催化化学 · 能源转换技术
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RSC Advances · 2018 ·Vol. 8 ·期 17 ·9211-9217 · IF 2.936

Mechanisms of partial hydrogen sorption reversibility in a 3NaBH4/ScF3 composite

Ning Zhao,Jianxin Zou,Xiaoqin Zeng,Wenjiang Ding

A new hydrogen storage composite containing NaBH4 and a 3d transition metal fluoride, 3NaBH4/ScF3, was synthesized via ball milling. The composite shows no reaction during milling and its dehydriding process can be divided into three steps upon heating: (i) partial substitution of H− by F− in NaBH4 to form NaBHxF4−x at the early stage, releasing about 0.19 wt% of hydrogen; (ii) formations of Na3ScF6, NaBF4 and ScB2 through the reaction between NaBH4 and ScF3, with 2.52 wt% of hydrogen release and a dehydriding activation energy of 162.67 kJ mol−1 H2; (iii) further reaction of residual NaBH4 and Na3ScF6 to form NaF, B and ScB2, with a dehydriding activation energy of 169.37 kJ mol−1 H2. The total hydrogen release of the composite reaches 5.54 wt% at 530 °C. The complete dehydrided composite cannot be rehydrogenated while the products after the second dehydriding step can be hydrogenated with an absorption activation energy of 44.58 kJ mol−1 H2. These results demonstrate that by adding 3d transition metal fluorides into NaBH4, a partial reversibility in NaBH4 can be achieved.

CAS / MDL: 16940-66-2
研究领域: 材料科学 · 氢存储 · 能源材料
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Metal–Nonmetal One-Dimensional Electrocatalyst: AuPdP Nanowires for Ambient Nitrogen Reduction to Ammonia

Hongjing Wang,Dandan Yang,Songliang Liu,Shuli Yin,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang

The Au catalyst is attractive for electrochemical ammonia synthesis. The design of Au catalyst with favorable morphology and composition is significant for enhancing its performance. Herein, an effective and universal synthetic method is proposed to fabricate unique metal–nonmetal AuPdP nanowires (AuPdP NWs), which is simply performed by the solvothermal reaction of Au nanowires with Pd(PPh3)4. The facile hydrogen adsorption at Pd sites and weak binding to Au sites favor the selective hydrogenation of N2 to NH3. Moreover, phosphorus doping provides more sites for the nitrogen reduction reaction due to its rich valence electrons. Therefore, the AuPdP NWs exhibit superior electrocatalytic performance for electrochemical ammonia synthesis with high NH3 yield, faradic efficiency, and stability. The presented synthetic method provides an attractive strategy for the simultaneous incorporation of Pd and P into metallic catalysts with controlled morphology for various electrocatalytic applications.

研究领域: 材料科学 · 电催化 · 化学工程
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DALTON TRANSACTIONS · 2021 ·Vol. 50 ·期 7 ·2414-2425 · IF 4.39

0D ultrafine ruthenium quantum dot decorated 3D porous graphitic carbon nitride with efficient charge separation and appropriate hydrogen adsorption capacity for superior photocatalytic hydrogen evolution

Pengfei An,Weihao Zhu,Luying Qiao,Shichao Sun,Yuyan Xu,Deli Jiang,Min Chen,Suci Meng

Designing a Pt-alternative cocatalyst capable of dissociating HO–H bonds is of great significance yet challenging for the development of high-efficiency and cost-effective water splitting photocatalytic systems. In this study, we designed and constructed a 0D ultrafine ruthenium (U-Ru) quantum dot decorated 3D porous g-C3N4 (3DpCN) nanohybrid (U-Ru/3DpCN) for photocatalytic hydrogen evolution, in which the U-Ru quantum dots act as cocatalysts accelerating the surface proton reduction reaction, and the 3D porous architecture assembled by 2D ultrathin nanosheets inherits a short charge diffusion distance and has a large specific surface area. Owing to these structural and physicochemical merits, the optimal photocatalyst U-1Ru/3DpCN achieves a superior hydrogen evolution performance of 2945.47 μmol g−1 h−1 under visible light with a high apparent quantum efficiency (AQE) of 9.5% at 420 nm, which is close to Pt-cocatalyst/3DpCN and better than most reported co-catalysts/g-C3N4 photocatalytic systems. Experimental results indicate that the formed Schottky junction between U-Ru and 3DpCN contributes to efficient charge separation, and DFT calculations show that the Ru-cocatalyst/g-C3N4 system has an appropriate hydrogen adsorption Gibbs free energy (ΔGH*) of 0.24 eV, which are both responsible to improve the photocatalytic performance. This study provides a new way to develop excellent photocatalysts for hydrogen evolution by the integration of cost-effective Ru quantum dot cocatalysts with nanostructured semiconductors.

研究领域: 材料科学 · 能源化学 · 催化化学
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