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Nanomaterials · 2022 ·Vol. 12 ·期 11 ·1890 · IF 5.719

Highly Active Palladium-Decorated Reduced Graphene Oxides for Heterogeneous Catalysis and Electrocatalysis: Hydrogen Production from Formaldehyde and Electrochemical Formaldehyde Detection

Xiaogang Liu,Wenjie Chen,Xin Zhang

The exploitation of highly efficient and stable hydrogen generation from chemical storage of formaldehyde (FA) is of great significance to the sustainable development of the future. Moreover, developing an accurate, rapid, reliable, and cost-effective catalyst for electrochemical detection of FA in solution is appealing. Herein, we report rational construction of Pd nanoparticles decorated reduced graphene oxides (Pd/rGO) nanohybrids not only as robust catalysts to produce hydrogen from alkaline FA solution and but also electrocatalysts for electrochemical detection of FA. By optimizing the reaction parameters including FA concentration, NaOH concentration and reaction temperature, Pd/rGO with Pd loading of 0.5 wt% could exhibit a high hydrogen production rate of 272 mL g−1min−1at room temperature of 25 °C, which is 3.2 times that of conventional Pd NPs. In addition, as-prepared Pd/rGO nanohybrids modified glassy carbon (GC) electrodes are used as FA-detected electrochemical sensors. A sensitive oxidation peak with a current density of 8.38 mA/cm2was observed at 0.12 V (vs. Ag/AgCl) in 0.5 M NaOH containing 10 mM FA over Pd/rGO catalysts with Pd loading of 0.5 wt%. The results showed the prepared Pd/rGO nanocatalyst not only exhibited efficient and stable hydrogen production from alkaline FA solution but also had good electrocatalytic properties with respect to formaldehyde electrooxidation as a result of the synergistic effect of Pd NPs and rGO nanosheets.Keywords:palladium;graphene;hydrogen production;formaldehyde detection

研究领域: 材料科学 · 电化学
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ACS Sustainable Chemistry & Engineering · 2017 · IF 5.951

NiO Quantum Dot Modified TiO2 toward Robust Hydrogen Production Performance

Weizhao Hong,Yansong Zhou,Chade Lv,Zhonghui Han,Gang Chen

Quantum dots (QDs) have great potential to build heterojunctions for efficient photocatalytic hydrogen production because of the quantum size effects, whereas they are limited by the rigorous preparation. Herein, we report a facile sacrificial coating strategy toward the construction of the NiO QDs/TiO2 heterojunction. Shorter transmission distance of carriers and higher crystallinity between NiO QDs and TiO2 substrate are achieved to minimize the recombination of photoinduced electrons and holes. As a result, excellent performance of 1.35 mmol h–1 g–1 over the NiO QDs/TiO2 sample is achieved, which is 37 times higher than that of NiO/TiO2 and 56 times higher than that of pure TiO2. Furthermore, this is one of the best performances reported in heterojunctions made of NiO and TiO2.

研究领域: 材料科学 · 能源科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

In-situ constructing ZnIn2S4@In(OH)3@CdS heterostructure for efficient photocatalytic H2 generation under visible light irradiation

Ligang Ma,Chao Lin,Wenjun Jiang,Le Xu,Yujie Shao,Tianyu Zhu,Ting Zhao,Xiaoqian Ai,Xiaoshan Wu

In the face of energy scarcity and environmental degradation, photocatalysis emerges as a green and highly efficient method to convert solar energy into a renewable energy source . In this study, CdS nanoparticles were successfully grown in situ along the edges of ZnIn 2 S 4 nanosheets using ultrasound during the synthesis process and the second phase precipitation of In(OH) 3 appeared in the process of preparation. Optimal Cd and S ratios resulted in ZnIn 2 S 4 @In(OH) 3 @CdS heterojunction exhibiting remarkable photocatalytic H 2 production performance compared to standalone ZnIn 2 S 4 and CdS. The internal heterojunction interface within the composite naturally generates an electric field, enhancing carrier separation and facilitating their transport. Additionally, the inclusion of In(OH) 3 further expedites carrier extraction. Ultimately, the mechanism behind the photocatalytic H 2 production was elucidated using the Z-scheme mechanism. This work introduced a novel approach to fabricating multifunctional photocatalysts , presenting a fresh perspective in their design and preparation.

研究领域: 材料科学 · 能源化学
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ELECTROCHIMICA ACTA · 2021 · IF 6.901

Ultrathin Ti2NTx MXene-wrapped MOF-derived CoP frameworks towards hydrogen evolution and water oxidation

Hui Zong,Ruijuan Qi,Ke Yu,Ziqiang Zhu

Hydrogen evolution is of great significance for reducing carbon emissions and realizing carbon-neutral. Hydrogen evolution reaction (HER) by water splitting has no carbon emissions and pollution, but it is still necessary to reduce cost and enhance catalytic activity. Herein, we report an ultra-thin Ti 2 NT x MXene-wrapped metal-organic frameworks (MOFs)-derived CoP composite (Ti 2 NT x @MOF-CoP), which is a bifunctional catalyst with low cost and high activity. We synthesize the Ti 2 NT x @MOF-CoP composite by phosphating the precursor ZIF-67 self-assembled with Ti 2 NT x MXene nanosheets. The Ti 2 NT x @MOF-CoP electrode shows competitive hydrogen evolution performance in a wide pH-range (current density of 10 mA cm −2 ) and has a low overpotential ( η ) of 112 mV in pH = 14 especially. The Ti 2 NT x @MOF-CoP electrode for OER also has a low η  = 241 mV at 50 mA cm −2 . Based on the bifunctional activity of Ti 2 NT x @MOF-CoP in alkaline, we set a dual-electrode configuration for HER and OER. It has a bias of 1.61 V at 10 mA cm −2 , with impressive catalytic stability during a 20 h measurement. MOFs-derived CoP has a large specific surface area and strong catalytic activity. Ti 2 NT x as a novel member of the MXene family not only can increase the active sites, but also can improve the stability of heterojunction catalysts. It reveals that the Ti 2 NT x @MOF-CoP composite has great potential in hydrogen evolution and water oxidation, thus reducing carbon emissions and protecting the environment.

研究领域: 材料科学 · 能源化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

ZnIn2S4 supported carbon dots/Ni3P hybrid for efficient photothermal catalytic hydrogen production from water

Juan Jia,Xiaomin Guo,Ying Tang,Wenjing Zeng,Hui Zeng,Zebao Rui

Construction of efficient and economically controllable catalysts for photocatalytic hydrogen production to relieve environmental and energy pressures remains an ongoing challenge. Herein, indium zinc sulfide supported carbon dots (CDs) and Ni 3 P hybrid (CDs/Ni 3 P/ZnIn 2 S 4 ) is designed as a robust catalyst for photothermal catalytic hydrogen production by water splitting. The co-introduction of CDs/Ni 3 P on ZnIn 2 S 4 as electron acceptors effectively enhances the photon harvest capacity and separation efficiency of photogenerated charges, and ultimately leads to excellent photothermal catalytic hydrogen production performance. The average hydrogen production rate of CDs/Ni 3 P/ZnIn 2 S 4 reaches 1880.78 μmol g −1  h −1 under 50 °C and full spectrum irradiation of 200 mW cm −2 , which is ∼8.8 times higher than the pristine ZnIn 2 S 4 and ranges among those over noble metal catalysts. Such a work provides a reliable route for the design of non-precious photothermal catalysts for photocatalytic hydrogen production.

研究领域: 材料科学 · 能源科学
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VACUUM · 2021 · IF 3.627

An active ZnxNi1-xS@Mo2C/carbon cloth electrode as efficient catalyst for water electrolysis

Zhiruo Shen,Changhua Xu,Sumin Wang,Jian Chen,Siqin Jia,Qiguan Wang

Electrolysis of water is a promising method for production of the green-energy hydrogen, which is commonly assisted by high powerful catalyst. At present, developing low-cost and highly efficient electrocatalysts has attracted increasing attention. Herein, a novel composited catalyst of Zn x Ni 1-x S@Mo 2 C loaded on conductive carbon cloth (Zn x Ni 1-x S@Mo 2 C/CC) is successfully prepared by the hydrothermal method . Due to the abundant active sites of defect structures induced by the surface engineering, the prepared Zn x Ni 1-x S@Mo 2 C/CC shows outstanding electrocatalytic performances in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) of water splitting, with low overpotential of 230 mV and 150 mV at 10 mA cm −2 , respectively. The Zn x Ni 1-x S@Mo 2 C/CC as an OER/HER bifunctional catalyst for overall water splitting affords a stable voltage of 1.56 V @current density of 10 mA cm −2 . Moreover, the catalyst shows an outstanding stability after a series of electrochemical tests. This work expands the multi-field applications of carbon cloth-supported materials as efficient non-precious metal-based electrocatalysts , with great importance in sustainable energy-relative technologies.

研究领域: 材料科学 · 能源技术
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Oxophilic Ce single atoms-triggered active sites reverse for superior alkaline hydrogen evolution

Shen Fengyi,Zhang Zhihao,Wang Zhe,Ren Hao,Liang Xinhu,Cai Zengjian,Yang Shitu,Sun Guodong,Cao Yanan,Yang Xiaoxin,Hu Mingzhen,Hao Zhengping,Zhou Kebin

The state-of-the-art alkaline hydrogen evolution catalyst of united ruthenium single atoms and small ruthenium nanoparticles has sparked considerable research interest. However, it remains a serious problem that hydrogen evolution primarily proceeds on the less active ruthenium single atoms instead of the more efficient small ruthenium nanoparticles in the catalyst, hence largely falling short of its full activity potential. Here, we report that by combining highly oxophilic cerium single atoms and fully-exposed ruthenium nanoclusters on a nitrogen functionalized carbon support, the alkaline hydrogen evolution centers are facilely reversed to the more active ruthenium nanoclusters driven by the strong oxophilicity of cerium, which significantly improves the hydrogen evolution activity of the catalyst with its mass activity up to −10.1 A mg −1 at −0.05 V. This finding is expected to shed new light on developing more efficient alkaline hydrogen evolution catalyst by rational regulation of the active centers for hydrogen evolution.

CAS / MDL: 57-13-6
研究领域: 催化 · 材料科学 · 能源材料
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

“Like-Compatible-Like” Strategy for High-Performance H2-Sieving Mixed-Matrix Membranes with Intensified Filler-Polymer Interfaces

Fengting Yao,Ziheng Li,Yan Dai,Xuehua Ruan,Xiaohang Yang,Xiaobin Jiang,Wenji Zheng,Gaohong He

Metal organic frameworks (MOFs)-based mixed matrix membranes (MMMs) exhibit great prospects for H 2 purification. However, their further development is hindered by interfacial incompatibility and framework flexibility-induced selectivity loss. Inspired by the “like compatible like” principle, a fluorinated engineering strategy is developed by introducing isoelectronic −CF 3 groups into ZIF-9 (FZIF-9), achieving dual regulation of MOF-polyimide (6FDA-TFMB) interfaces and molecular sieving architecture. The −CF 3 functionalization synergistically enhances interfacial compatibility through dipole interactions (C═O···F−C), optimizes pore size (3.67 Å) to achieve size-exclusive H 2 /CH 4 separation. Meanwhile, it suppresses the dissolution and adsorption of CH 4 molecules by reducing the CH 4 adsorption capacity on FZIF-9 by 40% compared with ZIF-9. The FZIF-9/PI-20 wt.% MMM exhibits excellent improvements of 22.1% and 133.1% in H 2 permeability (159 Barrer) and H 2 /CH 4 selectivity (295) over ZIF-9/PI-20 wt.% MMM. Importantly, its selectivity is superior to state-of-the-art MOFs/6FDA-based MMMs, approaching the 2015 Robeson upper bound. This work establishes fluorine-mediated interface engineering as a universal strategy for advanced gas-separation membranes, particularly in H 2 /CH 4 separation.

研究领域: 化学工程 · 材料科学 · 膜技术 · 气体分离 · 纳米技术
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Nature Communications · 2018 ·Vol. 9 ·期 1 ·1-7 · IF 12.353

MXene molecular sieving membranes for highly efficient gas separation

Ding Li,Wei Yanying,Li Libo,Zhang Tao,Wang Haihui,Xue Jian,Ding Liang-Xin,Wang Suqing,Caro Jürgen,Gogotsi Yury

Molecular sieving membranes with sufficient and uniform nanochannels that break the permeability-selectivity trade-off are desirable for energy-efficient gas separation, and the arising two-dimensional (2D) materials provide new routes for membrane development. However, for 2D lamellar membranes, disordered interlayer nanochannels for mass transport are usually formed between randomly stacked neighboring nanosheets, which is obstructive for highly efficient separation. Therefore, manufacturing lamellar membranes with highly ordered nanochannel structures for fast and precise molecular sieving is still challenging. Here, we report on lamellar stacked MXene membranes with aligned and regular subnanometer channels, taking advantage of the abundant surface-terminating groups on the MXene nanosheets, which exhibit excellent gas separation performance with H 2 permeability >2200 Barrer and H 2 /CO 2 selectivity >160, superior to the state-of-the-art membranes. The results of molecular dynamics simulations quantitatively support the experiments, confirming the subnanometer interlayer spacing between the neighboring MXene nanosheets as molecular sieving channels for gas separation.

CAS / MDL: 7789-24-4
研究领域: 材料科学 · 化学工程 · 纳米技术
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Capacitance effect of ZnIn2S4 with delicate morphology control on photocatalytic hydrogen evolution

Dong Feng,Tingyuan Zhang,Jiajia Wang,Wei Wang,Keying Lin,Baojun Ma,Fuxiang Zhang

The capacitance effect of semiconductor photocatalysts for hydrogen production is significant; however, the intrinsic role of capacitance in relation to the morphologies of photocatalysts remains unclear. Herein, we designed three different morphologies of ZnIn 2 S 4 semiconductor material—spherical, bulk, and rod-like—to determine their capacitance. In this study, the small capacitance characteristics of spherical ZnIn 2 S 4 (0.363F/g) enabled photoelectrons to quickly transfer to the surface and participated in the photocatalytic hydrogen evolution reaction, leading to a photocatalytic activity of 159 μmol/h/g. When TiVAlC nanoparticle with M n+1 AX n (MAX) nanostructure was employed as efficient co-catalyst, TiVAlC/ZnIn 2 S 4 -S achieved an increased activity of 285 μmol/h/g at 420 nm, which was 1.75 times that of TiVAlC/ZnIn 2 S 4 -B and 2.39 times that of TiVAlC/ZnIn 2 S 4 -R. This enhanced performance was attributed to the synergistic effect of the high-efficiency semiconductor photocatalyst ZnIn 2 S 4 -S with small capacitance and the superior conductivity of the Mxene material TiVAlC.

CAS / MDL: 22519-64-8
研究领域: 材料科学 · 能源技术
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Frontiers of Chemical Science and Engineering · 2021 ·Vol. 15 ·期 6 ·1561-1571 · IF 4.204

Superior performance in visible-light-driven hydrogen evolution reaction of three-dimensionally ordered macroporous SrTiO3 decorated with ZnxCd1−xS

Quan Huiying,Qian Kejiang,Xuan Ying,Lou Lan-Lan,Yu Kai,Liu Shuangxi

It is of broad interest to develop emerging photocatalysts with excellent light-harvesting capacity and high charge carrier separation efficiency for visible light photocatalytic hydrogen evolution reaction. However, achieving satisfying hydrogen evolution efficiency under noble metal-free conditions remains challenging. In this study, we demonstrate the fabrication of three-dimensionally ordered macroporous SrTiO3 decorated with Zn x Cd 1 − x S nanoparticles for hydrogen production under visible light irradiation (λ > 420 nm). Synergetic enhancement of photocatalytic activity is achieved by the slow photon effect and improved separation efficiency of photogenerated charge carriers. The obtained composites could afford very high hydrogen production efficiencies up to 19.67 mmol·g −1 ·h −1 , with an apparent quantum efficiency of 35.9% at 420 nm, which is 4.2 and 23.9 times higher than those of pure Zn0.5Cd0.5S (4.67 mmol·g −1 ·h −1 ) and CdS (0.82 mmol·g −1 ·h −1 ), respectively. In particular, under Pt-free conditions, an attractive hydrogen production rate (3.23 mmol·g −1 ·h −1 ) was achieved, providing a low-cost and high-efficiency strategy to produce hydrogen from water splitting. Moreover, the composites showed excellent stability, and no obvious loss in activity was observed after five cycling tests.

研究领域: 材料科学 · 能源化学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2017 ·Vol. 19 ·期 38 ·25919-25926 · IF 4.123

Developing an efficient NiCo2S4 cocatalyst for improving the visible light H2 evolution performance of CdS nanoparticles

Junwen Peng,Junli Xu,Zhaoyu Wang,Zhengxin Ding,Sibo Wang

Developing efficient alternatives to the widely used Pt cocatalyst in photocatalytic H2O splitting is of great importance in view of large-scale production of clear H2 energy. Herein, we report the facile synthesis of NiCo2S4 and its first use as a highly active and cost-affordable cocatalyst to boost visible light H2 generation with the CdS semiconductor. The synthesized NiCo2S4/CdS composite materials are fully characterized by various techniques including X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray (EDX) spectroscopy, X-ray photoelectron spectroscopy (XPS), UV-Vis diffusion reflectance spectroscopy (DRS), and N2 adsorption measurements. With the optimized NiCo2S4/CdS composite sample, a high H2 generation rate of 137 μmol h−1 is obtained under visible light irradiation, which is more than 17 times higher than that of bare CdS material. The results of photoluminescence (PL) spectroscopy, transient photocurrent response and electrochemical impedance spectroscopy demonstrate the remarkably promoted migration and separation of photogenerated charge carriers over the heterostructured NiCo2S4/CdS material, thus leading to obviously enhanced photocatalytic performance. Moreover, a possible mechanism for the photocatalytic H2 evolution reaction is also proposed based on the observed results of activity evaluation and photoelectrochemical measurements.

研究领域: 材料科学 · 能源化学
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