Step 1: Concept Entropy ($S$) decreases when randomness decreases, typically when gas moles are consumed or gas converts to liquid/solid.
Step 2: Meaning A positive $\Delta S$ means increased randomness; a negative $\Delta S$ means decreased randomness.
Step 3: Analysis (A), (B), and (C) produce more gas moles than they consume, increasing entropy. In (D), 3 moles of gas combine to form 2 moles of liquid, leading to a significant loss of randomness.
Step 4: Conclusion Reaction (D) shows a decrease in entropy ($\Delta S < 0$).
Final Answer: (D)