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For decades, photolysis and photocatalysis have been touted as promising environment-benign and robust technologies to degrade refractory pollutants from water. However, extensive, large-scale engineering applications remain limited now. To facilitate the technology transfer process, earlier reviews have advocated to developing more cost-effective and innocuous materials, maximizing efficiency of photon usage, and optimizing photoreactor systems, mostly from material and reactor improvement perspectives. However, there are also some fundamental yet critical chemistry issues in photo(cata)lysis processes demanding more in-depth understanding and more careful consideration. Hence, this review summarizes some of these challenges. Of them, the first and paramount issue is the interference of coexisting compounds, including dissolved organic matter, anions, cations, and spiked additives. Secondly …