Cu/Mg-MOF-74具有比表面积高、微孔结构和碱金属活性位点可调、CO₂吸附性能及光催化活性优良等优点, 但其Cu与Mg物质的量比(简称: Cu/Mg比)对烟气中CO₂吸附选择性影响机制尚不清晰。本研究采用溶剂热法合成了不同Cu/Mg比的Cu/Mg-MOF-74, 表征了其CO₂光催化性能、CO₂和N₂吸附量及孔结构, 计算了Cu/Mg-MOF-74的CO₂吸附选择性, 并分析了Cu/Mg比对吸附量、选择性影响机制。结果表明：随着Cu/Mg比减小, Cu/Mg-MOF-74光催化CO₂还原为CO和H₂的活性先增后减, 当Cu/Mg比为0.6/0.4时, 其光催化还原CO和H₂产率最大, 分别为10.65和5.41 μmol·h⁻¹·g_cat⁻¹(1 MPa, 150 ℃); 随着Cu/Mg比减小, CO₂、N₂在Cu/Mg-MOF-74上的吸附量增加, 且CO₂吸附量增加显著, 当Cu/Mg比为0.1/0.9时, 其CO₂、N₂吸附量最大, 分别为9.21、1.49 mmol·g⁻¹(273.15 K, 100 kPa); 随着Cu/Mg比减小, Cu/Mg-MOF-74的微孔(d₁≥0.7 nm)、超微孔(d₂<0.7 nm)的面积、体积均增加, 当Cu/Mg比为0.22/0.78时, 其微孔、超微孔的面积、体积均大于Mg-MOF-74; 其选择性随Cu/Mg比减小和CO₂浓度增大而改善。CO₂在Cu/Mg-MOF-74上的吸附作用包括微孔填充和Mg²⁺化学吸附, 微孔体积是影响其吸附性能的关键。调整Cu/Mg比可调控Cu/Mg-MOF-74的孔结构、CO₂吸附量和选择性。

甲烷是对全球温升贡献仅次于二氧化碳的温室气体, 且其全球增温潜势是CO₂的80倍以上。在全球变暖和大气中甲烷含量不断增长的背景下, 完全催化氧化大气甲烷对于减缓温室效应和全球变暖具有重要价值。然而, 由于甲烷具有较高的结构稳定性, 在温和条件下将其催化氧化一直面临巨大的挑战。本文综述了近年来甲烷完全氧化在热催化、光催化以及光热协同催化三种反应条件下的研究进展, 热催化中高温增大了能耗并加速了催化剂的失活, 开发低温反应条件下的催化剂已经成为甲烷完全热催化的重点; 光催化提供了一种常温常压条件下利用光能氧化甲烷的方法, 但是相对热催化来说反应速率较低; 光热协同催化在光能和热能的协同作用下, 可实现温和条件下的甲烷高效完全催化氧化, 表现出潜在的应用前景。本文就三种反应催化剂的发展进行综述, 系统分析了不同反应的原理, 以及不同反应条件下甲烷完全催化氧化的优势与不足, 同时总结了催化氧化甲烷所面临的挑战, 并提供潜在的解决方案, 期望为今后的甲烷氧化研究提供借鉴。

In recent years, the treatment of agricultural wastewater has been an important aspect of environmental protection. The purpose of photocatalytic technology is to degrade pollutants by utilizing solar light energy to stimulate the migration of photocarriers to the surface of photocatalysts and occur reduction-oxidation reaction with pollutants in agricultural wastewater. Photocatalytic technology has the characteristics of high efficiency, sustainability, low-energy and free secondary pollution. It is an environmental and economical method to recover water quality that only needs sunlight. In this paper, the mechanism and research progress of photocatalytic removal of heavy metal ions and antibiotics from agricultural water pollution were reviewed by combining photocatalytic degradation process with agricultural treatment technology. The mechanism of influencing factors of photocatalytic degradation efficiency was discussed in detail and corresponding strategies were proposed, which has certain reference value for the development of photocatalytic degradation.

Plasmonics has aroused tremendous interest in photophysics, nanophotonics, and metamaterials. The extreme field concentration of plasmonics offers the ultimate spatial and temporal light control, single-particle detection, and optical modulation. Plasmon decay of metal nanostructures into hot carriers extends the application into photocatalysis, photodetectors, photovoltaics, and ultrafast nanooptics. The generated hot electron–hole pairs are transferred into adjacent dielectrics, well known to be more efficient than the hot carrier generation in dielectrics by direct photoexcitations. However, plasmon-induced hot-carrier-based devices are far from practical applications due to the low quantum yield of hot carrier extraction. Emergent challenges include low hot carrier generation efficiency in metals, rapid energy loss of hot carriers, and severe charge recombination at the metal/dielectric interface. In this review, we provide a fundamental insight into the hot carrier generation, transport, injection, and diffusion into dielectrics based on the steady-state and time-resolved spectroscopic studies as well as theoretical calculations. Strategies to enhance hot carrier generation in metals and electron transfer into dielectrics are discussed in detail. Then, applications based on hot carrier transfer are introduced briefly. Finally, we provide our suggestions on future research endeavors. We believe this review will provide a valuable overall physical picture of plasmon-induced hot carrier applications for researchers.