The size effects of metal catalysts have been widely investigated to optimize their catalytic activity and selectivity. However, the size-controllable synthesis of uniform supported metal nanoparticles without surfactants and/or additives remains a great challenge. Herein, we developed a green, surfactant-free, and universal strategy to tailor the sizes of uniform Pd nanoparticles on metal oxides by an electroless chemical deposition method via defect engineering of supports. The nucleation and growth mechanism suggest a strong electrostatic interaction between the Pd precursor and low-defective CeO2 and a weak reducing capacity for low-defective CeO2, resulting in small Pd nanoparticles. Conversely, large Pd nanoparticles were formed on a highly defective CeO2 surface. Combined with various ex situ and in situ characterizations, a higher intrinsic activity of Pd for the CO2-to-CO hydrogenation was found on large Pd nanoparticles with higher electron density owing to their stronger H2 dissociation ability and H-spillover effects, as well as the larger number of oxygen vacancies generated in situ for CO2 activation under hydrogenation conditions.
Border area is not only an important gateway for inland opening-up, but also an important part of completing the building of a moderately prosperous society and optimizing national urban spatial pattern in China. Due to the location, natural resources endowment, and traffic accessibility, the urbanization speed is relatively slow in border areas. Therefore, it is a special area that needs to pay close attention to, especially under the background of the Belt and Road Initiative and China's regional coordinated development program. Based on the county-level data from 2000 to 2015, this paper tries to analyze the spatio-temporal pattern of urbanization in 134 border counties, and applies geographical detector method to study the driving forces of urbanization in border areas. Conclusions are as follows: (1) From 2000 to 2015, urbanization rate in border areas has been lower than the national average, and the gap has been widening. Some border counties in southern Xinjiang, Tibet, northeast of Inner Mongolia, and Yunnan, are even facing the problem of population loss. (2) In the same period, urbanization rate in the northwestern and southwestern border is low, while their urbanization rate grows relatively faster comparing with other border counties; urbanization rate in Tibet border is the lowest and grows relatively slowly; urbanization rate in the northeastern and northern border is slightly higher, but it grows slowly or even stagnates. (3) Transportation and industry are the important driving forces of urbanization in border areas, while the driving forces of market is relatively weak. And there are obvious mutual reinforcements among the driving forces, while the effort and explanatory power of resource force increases obviously after interaction. (4) Urbanization rate in the northwestern and southwestern border areas grows relatively fast, with industrial force and transportation force, market force and administrative force as the main driving forces respectively. Tibet border area has the lowest urbanization rate and growth rate, as the driving force of urbanization with strong contribution has not yet formed in Tibet. In the northeastern and northern border areas, the contribution of transportation force to urbanization is greater than other forces, and its interaction with market and industry has obvious effects.
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