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61.
《中国化学快报》2020,31(4):988-991
Designing efficient electrocatalysts with low Pt loadings for hydrogen evolution reaction(HER) is urgently required for renewable and sustainable energy conversion.Here,we report a strategy that Pt nanoparticulates are spontaneously immobilized on porous MXene/MAX monolith as HER catalysts by utilizing the redox reaction between Ti_3C_2T_x MXene and [PtCl_4]~2 in H_2 PtCl_6 aqueous solution.By taking advantage of homogeneously distributed Pt nanoparticulates on highly electrically conductive porous Ti_3C_2T_x/Ti_3AlC_2 monolith,the as-prepared electrocatalysts show high catalytic performance for hydrogen evolution.Specifically,the binder-free electrocatalysts have Pt loadings as low as 8.9 μg/cm~2,with low overpotential of 43 mV at a curre nt density of 10 mA/cm~2 and low Tafel slope that three times lower than porous Ti_3C_2T_x/Ti_3AlC_2 without Pt loading.This strategy offers a new approach to constructing ultra-low Pt-loading HER catalysts on the basis of in situ redox reaction between noble metal ions and MXenes. 相似文献
62.
硫酸介质中Ti/SnO2/PbO2析氧阳极的研究 总被引:13,自引:0,他引:13
由于硫酸溶液具有高的电导、一般条件下性质稳定、价格相对低廉等优点,所以电化学合成大多在硫酸溶液中进行.阳极析氧是电化学合成不可避免的阳极过程.但因硫酸的强腐蚀性,以及从阳极析出的氧的强氧化性,使得能满足工业生产的阳极材料很缺乏.自1950年荷兰Hen... 相似文献
63.
基于构建的数字经济发展水平评价指标体系与2010~2018年全国30个省市(除西藏、港澳台)的面板数据,对中国数字经济发展水平的时空特征、动态演化与区域差异原因进行探究。研究发现:全国及三大区域的数字经济发展水平均呈现稳步上升态势,并伴有明显的空间相关性、空间集聚性和区域差异性,且东部相较于中西部区域内差异更大。数字经济发展速度动态演化显示,整体上中国各省市数字化发展水平变化速度状态表现为上升趋势,相较于中西部,东部拥有更大的速度变化状态。地区前期数字化基础、经济发展的一阶滞后、政府科技投入均会促进区域数字经济的发展,对外开放水平会抑制数字经济发展,地区规模对数字经济的影响表现为非线性。此外,不同线性影响因素在不同区域内对数字经济发展水平具有不同的影响力。 相似文献
64.
Qin Yang Bingqing Ge Pei Yuan Shuting Luo Hongwei Zhang Zhengyu Zhao Jiujun Zhang Shidong Wang Xiaojun Bao Xiangdong Yao 《Advanced functional materials》2023,33(25):2214588
Electrocatalytic hydrogenation (ECH) is a burgeoning strategy for the sustainable utilization of hydrogen. However, how to effectively suppress the competitive hydrogen evolution reaction (HER) is a big challenge to ECH catalysis. In this study, amine (NH2 R)-coordinated Pd nanoparticles loaded on carbon felt (Pd@CF) as a catalyst is successfully synthesized by a one-step solvothermal reduction method using oleylamine as the reducing agent. An exceptional ECH reactivity on benzaldehyde is achieved on the optimal Pd@CF catalyst in terms of a high conversion (89.7%) and selectivity toward benzyl alcohol (89.8%) at −0.4 V in 60 min. Notably, the Faradaic efficiency for producing benzyl alcohol is up to 90.2%, much higher than that catalyzed by Pd@CF-without N-group (41.1%) and thecommercial Pd/C (20.9%). The excellent ECH performance of Pd@CF can be attributed to the enriched electrons on Pd surface resulted from the introduction of NH2 R groups, which strengthens both the adsorption of benzaldehyde and the adsorbed hydrogen (Hads) on Pd, preventing the combination of Hads to form H2, that is, inhibiting the HER. This study gives a new insight into design principles of highly efficient electrocatalysts for the hydrogenation of unsaturated aldehydes molecules. 相似文献
65.
Saurav Ch Sarma Jesús Barrio Alexander Bagger Angus Pedersen Mengjun Gong Hui Luo Mengnan Wang Silvia Favero Chang-Xin Zhao Qiang Zhang Anthony Kucernak Maria-Magdalena Titirici Ifan E. L. Stephens 《Advanced functional materials》2023,33(41):2302468
The electrochemical CO2 reduction reaction (CO2RR) to value-added chemicals with renewable electricity is a promising method to decarbonize parts of the chemical industry. Recently, single metal atoms in nitrogen-doped carbon (MNC) have emerged as potential electrocatalysts for CO2RR to CO with high activity and faradaic efficiency, although the reaction limitation for CO2RR to CO is unclear. To understand the comparison of intrinsic activity of different MNCs, two catalysts are synthesized through a decoupled two-step synthesis approach of high temperature pyrolysis and low temperature metalation (Fe or Ni). The highly meso-porous structure results in the highest reported electrochemical active site utilization based on in situ nitrite stripping; up to 59±6% for NiNC. Ex situ X-ray absorption spectroscopy (XAS) confirms the penta-coordinated nature of the active sites. The catalysts are amongst the most active in the literature for CO2 reduction to CO. The density functional theory calculations (DFT) show that their binding to the reaction intermediates approximates to that of Au surfaces. However, it is found that the turnover frequencies (TOFs) of the most active catalysts for CO evolution converge, suggesting a fundamental ceiling to the catalytic rates. 相似文献
66.
Xin Ding Run Jiang Jialin Wu Minghui Xing Zelong Qiao Xiaofei Zeng Shitao Wang Dapeng Cao 《Advanced functional materials》2023,33(47):2306786
Developing low-cost and high-efficient bifunctional catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is greatly significant for water electrolysis. Here, Ni3N-CeO2/NF heterostructure is synthesized on the nickel foam, and it exhibits excellent HER and OER performance. As a result, the water electrolyzer based on Ni3N-CeO2/NF bifunctional catalyst only needs 1.515 V@10 mA cm−2, significantly better than that of Pt/C||IrO2 catalysts. In situ characterizations unveil that CeO2 plays completely different roles in HER and OER processes. In situ infrared spectroscopy and density functional theory calculations indicate that the introduction of CeO2 can optimizes the structure of interface water, and the synergistic effect of Ni3N and CeO2 improve the HER activity significantly, while the in situ Raman spectra reveal that CeO2 accelerates the reconstruction of OV (oxygen vacancy)-rich NiOOH for boosting OER. This study clearly unlocks the different catalytic mechanisms of CeO2 for boosting the HER and OER activity of Ni3N for water splitting, which provides the useful guidance for designing the high-performance bifunctional catalysts for water splitting. 相似文献
67.
Yeshu Tan Jianrui Feng Haobo Dong Longxiang Liu Siyu Zhao Feili Lai Tianxi Liu Ying Bai Ivan P. Parkin Guanjie He 《Advanced functional materials》2023,33(4):2209967
Platinum (Pt) is regarded as a promising electrocatalyst for hydrogen evolution reaction (HER). However, its application in an alkaline medium is limited by the activation energy of water dissociation, diffusion of H+, and desorption of H*. Moreover, the formation of effective structures with a low Pt usage amount is still a challenge. Herein, guided by the simulation discovery that the edge effect can boost local electric field (LEF) of the electrocatalysts for faster proton diffusion, platinum nanocrystals on the edge of transition metal phosphide nanosheets are fabricated. The unique heterostructure with ultralow Pt amount delivered an outstanding HER performance in an alkaline medium with a small overpotential of 44.5 mV and excellent stability for 80 h at the current density of −10 mA cm−2. The mass activity of as-prepared electrocatalyst is 2.77 A mg−1Pt, which is 15 times higher than that of commercial Pt/C electrocatalysts (0.18 A mg−1Pt). The density function theory calculation revealed the efficient water dissociation, fast adsorption, and desorption of protons with hybrid structure. The study provides an innovative strategy to design unique nanostructures for boosting HER performances via achieving both synergistic effects from hybrid components and enhanced LEF from the structural edge effect. 相似文献
68.
Kexin Wang Junhui Cao Xiaoxuan Yang Xiahan Sang Siyu Yao Rong Xiang Bin Yang Zhongjian Li Thomas O'Carroll Qinghua Zhang Lecheng Lei Gang Wu Yang Hou 《Advanced functional materials》2023,33(16):2212321
Designing hydrogen evolution reaction (HER) electrocatalysts for facilitating its sluggish adsorption kinetics is crucial in generating green hydrogen via sustainable water electrolysis. Herein, a high-performance ultra-low Ruthenium (Ru) catalyst is developed consisting of atomically-layered Ru nanoclusters with adjacent single Ru sites, which executs a bridging-Ru-H activation strategy to kinetically accelerate the HER elementary steps. Owing to its optimal electronic structure and unique adsorption configuration, the hybrid Ru catalyst simultaneously displayed a drastically reduced overpotential of 16 mV at 10 mA cm−2 as well as a low Tafel slope of 35.2 mV dec−1 in alkaline electrolyte. When further coupled with a commercial IrO2 anode catalyst, the ensembled anion-exchange membrane water electrolyzer achievs a current density of 1.0 A cm−2 at a voltage of only 1.70 Vcell. In situ spectroscopic analysis verified that Ru single atom and atomically-layered Ru nanoclusters in the hybrid materials play a critical role in facilitating water dissociation and weakening *H adsorption, respectively. Theoretical calculations further elucidate the underlaying mechanism, suggesting that the dissociated proton at the single atom Ru site orients itself adjacently with Ru nanoclusters in a bridged structure through targeted charge transfer, thus promoting Volmer-Heyrovsky dynamics and boosting the HER activity. 相似文献
69.
Jiafeng Zhu Qingyuan Bi Yinghao Tao Wenyao Guo Jinchen Fan Yulin Min Guisheng Li 《Advanced functional materials》2023,33(15):2213131
Designing and developing visible-light-responsive materials for solar to chemical energy is an efficient and promising approach to green and sustainable carbon-neutral energy systems. Herein, a facile in situ growth hydrothermal strategy using Mo-modified ZnIn2S4 (Mo-ZIS) nanosheets coupled with NiTiO3 (NTO) microrods to synthesize multifunctional Mo-modified ZIS wrapped NTO microrods (Mo-ZIS@NTO) photocatalyst with enhanced interfacial electric field (IEF) effect and typical S-scheme heterojunction is reported. Mo-ZIS@NTO catalyst possesses wide-spectrum light absorption properties, excellent visible light-to-thermal energy effect, electron mobility, charges transfer, and strong IEF and exhibits excellent solar-to-chemical energy conversion for efficient visible-light-driven photocatalytic hydrogen evolution. Notably, the engineered Mo1.4-ZIS@NTO catalyst exhibits superior performance with H2 evolution rate of up to 14.06 mmol g−1 h− 1 and the apparent quantum efficiency of 44.1% at 420 nm. The scientific explorations provide an in-depth understanding of microstructure, S-scheme heterojunction, enhanced IEF, Mo-dopant facilitation effect. Moreover, the theoretical simulations verify the critical role of Mo element in promoting the adsorption and activation of H2O molecules, modulating the H adsorption behavior on active S sites, and thus accelerating the overall catalytic efficiency. The photocatalytic hydrogen evolution mechanism via S-scheme heterojunction with adjustable IEF regulation over Mo1.4-ZIS@NTO is also demonstrated. 相似文献
70.
Yanying Li Qiwen Zhang Xiaoran Zhao Haofei Wu Xinyao Wang Yuqiao Zeng Qing Chen Mingwei Chen Pan Liu 《Advanced functional materials》2023,33(17):2370105
The development of low-cost and effective oxygen evolution reaction (OER) electrocatalysts to expedite the slow kinetics of water splitting is crucial for increasing the efficiency of energy conversion from electricity to hydrogen fuel. Herein, 3D bicontinuous nanoporous Co@CoO/RuO2 composites with tunable sizes and chemical compositions are fabricated by introducing vapor phase dealloying of cobalt-based alloys. The influence of physical parameters on the formation of nanoporous Co substrates with various feature ligament sizes is systematically investigated. The CoO/RuO2 shell is constructed by integrating a thin layer of RuO2 on the inner surface of nanoporous Co, where the CoO interlayer is formed by annealing oxidization. The composite catalyst delivers an ultralow overpotential of 198 mV at 10 mA cm−2, Tafel slope of 57.1 mV dec−1, and long-term stability of 50 h. The superior OER activity and fast reaction kinetics are attributed to charge transfer through the coupling of Co O Ru bonds at the interface and the excellent nanopore connectivity, while the durability originates from the highly stable CoO/RuO2 interface. 相似文献