The enzyme nitrogenase inspires the development of novel photocatalytic and electrocatalytic systems that can drive nitrogen reduction with water under similar low‐temperature and low‐pressure conditions. While photocatalytic and electrocatalytic N 2 fixation are emerging as hot new areas of fundamental and applied research, serious concerns exist regarding the accuracy of current methods used for ammonia detection and quantification. In most studies, the ammonia yields are low and little consideration is given to the effect of interferants on NH 3 quantification. As a result, NH 3 yields reported in many works may be exaggerated and erroneous. Herein, the advantages and limitations of the various methods commonly used for NH 3 quantification in solution (Nessler's reagent method, indophenol blue method, and ion chromatography method) are systematically explored, placing particular emphasis on the effect of interferants on each quantification method. Based on the data presented, guidelines are suggested for responsible quantification of ammonia in photocatalysis and electrocatalysis.

An organic–inorganic perovskite is comprised of an organic cation (CH3NH3+, FAI, or Cs), a metal cation (Pb2+or Sn2+) and a halide (I−, Cl−, or Br−) molecule.

Layered double hydroxide (LDH) nanosheets show good activity in a wide range of photoreactions, with this activity being generally attributable to an abundance of surface oxygen vacancies or coordinatively unsaturated metal cations in the nanosheets which serve as active sites for reactant adsorption and activation. Recently, LDH nanosheets have been shown to be very effective for photocatalytic N2 reduction to NH3 using water as the reducing agent. Herein, it is demonstrated that a simple pretreatment of ZnCr‐LDH, ZnAl‐LDH, and NiAl‐LDH nanosheets with aqueous NaOH can greatly enhance the concentration of oxygen vacancies and low coordination metal centers in the nanosheets, thus significantly enhancing their photocatalytic activity for N2 reduction to NH3 under UV–vis irradiation (without the need for added sacrificial agents or cocatalysts). The facile alkali etching strategy introduced here is expected to be widely adopted in the future development of high‐performance LDH photocatalysts for ammonia production and other challenging chemical transformations (e.g., CO2 reduction and water splitting).