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太原理工大学 化学与化工学院,山西 太原 030024
Received:27 January 2026,
Revised:2026-02-27,
Online First:02 June 2026,
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贾志怡,刘红艳,夏利民等.MoFe/氮化物的磁控溅射制备及其合成氨性能研究[J].低碳化学与化工,
JIA Zhiyi,LIU Hongyan,XIA Limin,et al.Study on magnetron sputtering preparation of MoFe/nitrides and their ammonia synthesis performances[J].Low-Carbon Chemistry and Chemical Engineering,
贾志怡,刘红艳,夏利民等.MoFe/氮化物的磁控溅射制备及其合成氨性能研究[J].低碳化学与化工, DOI:10.12434/j.issn.2097-2547.20260043.
JIA Zhiyi,LIU Hongyan,XIA Limin,et al.Study on magnetron sputtering preparation of MoFe/nitrides and their ammonia synthesis performances[J].Low-Carbon Chemistry and Chemical Engineering, DOI:10.12434/j.issn.2097-2547.20260043.
氮空位与功函数是调
控非金属氮化物催化合成氨性能的关键因素,但传统化学合成法难以精准控制。为探究氮空位浓度与功函数如何调控合成氨催化性能,采用绿色高效的射频磁控溅射法,以高纯N
2
为溅射气体,在SiO
2
衬底上制备了氮化硼(BN)、氮化碳(CN)和氮化硼碳(BCN)3种非金属氮化物薄膜,并进一步沉积MoFe合金制备了复合催化体系(MoFe/BN、MoFe/CN和MoFe/BCN)。运用EPR、UPS和XPS等表征方法,对氮空位浓度、功函数及催化剂表面电子态进行了分析,并在微型固定床反应器中评价了催化剂热催化合成氨性能。结果表明,磁控溅射制备的3种氮化物均富含氮空位(
g
因子 ≈ 2.004),功函数分别为2.47 eV(CN)、2.53 eV(BCN)和4.46 eV(BN)。在800 ℃、环境气压条件下,MoFe/CN的氨生成速率达72.98 μg/(g·h),显著高于MoFe/BN、MoFe/BCN及纯MoFe。XPS结果证实了CN载体通过强金属-载体相互作用向MoFe转移电子,将Mo、Fe还原至更低氧化态。综上,磁控溅射技术可实现氮空位与功函数的协同调控,低功函数CN载体通过界面电子转移优化MoFe活性中心的电子结构,从而提升了合成氨反应性能。
Nitrogen vacancies and work function are key factors regulating the catalytic performance of non-metal nitrides for ammonia synthesis
whereas precise control by conventional chemical synthesis methods remains difficult. To investigate how nitrogen vacancy concentration and work function regulate the catalytic performance of ammonia synthesis
green and efficient radio frequency magnetron sputtering was employed to prepare boron nitride (BN)
carbon nitride (CN) and boron carbon nitride (BCN) non-metal nitride thin films on SiO
2
substrates using high-purity N
2
as the sputtering gas
and MoFe alloy was further deposited to construct composite catalytic systems (MoFe/BN
MoFe/CN and MoFe/BCN). EPR
UPS and XPS characterization methods were employed to analyze the nitrogen vacancy concentration
work function and surface electronic states of the catalysts
and the thermocatalytic ammonia synthesis performance was evaluated in a micro-fixed-bed reactor. The results show that the three nitrides prepared by magnetron sputtering are all rich in nitrogen vacancies (
g
-factor ≈ 2.004)
and their work functions are 2.47 eV (CN)
2.53 eV (BCN) and 4.46 eV (BN)
respectively. Under 800 ℃ and ambient pressure conditions
the ammonia formation rate of MoFe/CN reaches 72.98 μg/(g·h)
which is significantly higher than those of MoFe/BN
MoFe/BCN and pure MoFe. XPS resul
ts confirm that the CN support transfers electrons to MoFe through strong metal-support interactions
reducing Mo and Fe to lower oxidation states. In summary
magnetron sputtering technology can realize the synergistic regulation of nitrogen vacancies and work function
and the low-work-function CN support optimizes the electronic structure of MoFe active centers through interfacial electron transfer
thereby improving the ammonia synthesis performance.
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